Research ArticleEncapsulation of Moringa oleifera Extract in Ca-AlginateChocolate Beads Physical and Antioxidant Properties

Olga Kaltsa Aggeliki Alibade Eleni Bozinou Dimitris P Makris and Stavros I Lalas

Department of Food Science amp Nutrition University of essaly Terma N Temponera Street GR-43100 Karditsa Greece

Correspondence should be addressed to Stavros I Lalas slalasuthgr

Received 27 February 2021 Revised 6 May 2021 Accepted 28 May 2021 Published 4 June 2021

Academic Editor Walid Elfalleh

Copyright copy 2021 Olga Kaltsa et al is is an open access article distributed under the Creative Commons Attribution Licensewhich permits unrestricted use distribution and reproduction in any medium provided the original work is properly cited

e aim of the present study was to evaluate the physical and antioxidant properties of chocolate alginate beads containingMoringaoleifera leaf extract (MLE) produced with ecofriendly solvent extraction technology (Deep Eutectic Solvents) e concentration ofMLE incorporated was 0 2 4 and 6 ww and hardening time for ionotropic gelation with CaCl2 solution was 2 8 or 20minFreshly prepared beads were evaluated for their geometric (area perimeter ferret diameter circularity roundness) color (CIE Llowast alowastand blowast and chroma) and antioxidant properties (total phenolic content and percentage inhibition of DPPHbull radical) Increasing theMLE concentration resulted in beads smaller in size and more spherical whereas hardening time only affected their circularity MLEconcentration had also a profound effect on color and antioxidant properties of the beads As the concentration ofMLE increased thebeads appeared lighter and their chroma increased e radical scavenging activity was ameliorated by the MLE concentrationincrease for samples hardened for 8 and 20min whereas it was unaffected for those at 2mine hardening time on the contrary didnot affect the inhibition of DPPHbull values regardless of the amount of extract added

1 Introduction

Within the last decade there is an increasing interest infunctional health-promoting foods from all three partsinvolved science food industry and consumers As mostprocesses during food preparation contribute to significantdegradation of vital compounds (phytochemicals antioxi-dants vitamins) and probiotics a significant number oftechniques have been developed focusing on the encapsu-lation of these sensitive constituents In addition the en-capsulation of bioactive ingredients offers the advantage oftargeted delivery and controlled release in the human gas-trointestinal tract which increase their bioefficiency [1]Only to begin with nano-microemulsification multipleemulsion formation liposome entrapment spray dryinglyophilization ionotropic gelation and coacervation rep-resent the most widely known [2] Emerging electro-hydrodynamic techniques like electrospinning andelectrospraying are also promising tools for fabrication offibrous or sphere-shaped vehicles [2 3]

Moringa oleifera Lam (drumstick tree) is a plant nativeto northern India largely appreciated for its uses in tradi-tional medicine Although every part of the tree is usefulthere is growing interest for its leaf extract because of thehigh concentrations in certain antioxidant compounds suchas vitamin E ascorbic acids β-carotene quercetin phenolicacids and flavonoids [4ndash6] A plethora of in vivo and in vitrostudies provide significant evidence on the prophylacticeffect against common diseases including Alzheimerrsquosatherosclerosis diabetes and neoplasms [7] With respect toits antioxidant properties an appreciable number of studieshave been conducted within the last few years [8ndash10]Moringa oleifera extract has also been successfully encap-sulated using different techniques in various systems such aselectrospun nanofibers [11] microemulsions [12] phyto-somes [13] and spray-dried capsules [14]

e ionotropic gelation of alginates in the presence ofCa2+ orMg2+ by the cross-linkingmechanism is a very usefulaffordable encapsulation technique for food and nonfoodapplications that offers among others advantages such as

HindawiJournal of Food QualityVolume 2021 Article ID 5549873 9 pageshttpsdoiorg10115520215549873

biodegradability biocompatibility and implementationsimplicity [15] In addition the size shape and controlledrelease of encapsulated materials can be easily tailored tomeet the needs of specific applications ie drugs ornutraceuticals is can be achieved by altering the chemicalstructure of the encapsulant procedure variables andmatrixcomposition [16ndash18] As a consequence the encapsulation ofwidely used herbal extracts rich in polyphenols (olive leafpomegranate beetroot and cocoa) in Ca-alginate hydrogelshas been the subject of an appreciable number of studies[19ndash22] Wine by-product extract [23] and medicinal ex-tracts of Plectranthus species have also been successfullyencapsulated in similar systems [24 25]

e limited reports that exist on encapsulation ofMoringa leaf extract (MLE) in alginate beads focus on theremoval of heavy metals [26 27] or their bactericidal activity[28] and lack vital information related to their physicalantioxidant properties and possible application in food

erefore the main scope of this work was to encap-sulate MLE prepared with the use of deep eutectic solvents(DES) in chocolate-flavored alginate beads via ionic gelationto enhance their antioxidant capacity e effect of selectedparameters (curing time and extract concentration) on thephysical and antioxidant properties of the alginate beads isdiscussed

2 Material and Methods

21 Materials Folin-Ciocalteu reagent 11-diphenyl-2-picryl-hydrazyl (DPPHbull) glacial acetic acid CaCl2 andCaCO3 were purchased from Sigma-Aldrich (St Louis MOUSA) Gallic acid hydrate and Folin-Ciocalteu was fromPanreac (Barcelona Spain) Cocoa butter and whey proteinconcentrate (80 in protein) were kind donations fromCocoowa (essaloniki Greece) and Tyrokomiki KarditsasSA (Karditsa Greece) respectively Cocoa powder wasobtained from a local store Alginate powder was donated byKenfood SA (Keratsini Greece) MLE was prepared underthe optimum conditions previously reported by Zam et al[20] using DES In the same study a detailed analysis of thechemical properties of the MLE (total polyphenol and fla-vonoid content antiradical activity ferric reducing powerand polyphenolic profile by LC-MS and HPLC) is provided

22 Methods

221 Preparation of Chocolate Beads Containing MLEe chocolate used to formulate the MLE-containing algi-nate beads was prepared according to the main methodologyfor chocolate manufacture that involves four differentphases dry mixing grinding conching and molding [29] Itcontained 36 ww cocoa butter 32 ww sugar 12 wwcocoa powder and 20 ww whey protein concentrate

Finally alginate chocolate beads were prepared as fol-lows sodium alginate powder (2 g) was dispersed in doubledistilled water (60 g) containing 20 g chocolate 05 g po-tassium sorbate and 05 g potassium benzoate e mix wasvigorously stirred for 45min at 500 rpm50degC e alginatedispersion was left to cool at ambient temperature MLE was

added at 0 2 4 and 6 ww concentration and water wastopped up to 100 g for each formulation e spherificationof the final alginate dispersion was carried out with plasticpipettes and the dripping procedure in CaCl2 solution (2ww) lasted 3min e distance between the pipette nozzleand the surface of the CaCl2 solution was 2 cm e beadswere maintained in the CaCl2 solution to gel for 2 8 or20min and afterward filtered and washed with doubledistilled water to remove excess calcium and stop hardeningCuring time intervals were selected with preliminary testingin order to correspond to different types of texture samplescured for 2min were very soft and easily broken upon slightpressure with the tongue samples of 8min represent morecohesive beads and samples of 20min were hard spheresthat required extensive chewing to disintegrate All sampleswere prepared and analyzed at least in triplicate

222 Chocolate Beads Particle Size e particle size of thebeads was estimated by means of image analysis Photos ofthe beadsrsquo samples were captured with a digital cameracoupled with a computer e free license image analysissoftware ImageJ v 146r (httpsimagejnihgovijindexhtml) was used to calculate the geometric properties ofthe beads area (mm2) ferret diameter (mm) perimeter(mm) roundness (minus) and circularity (minus) For each mea-surement approximately 200 beads were measured perbatch

223 Color Measurement Color properties of chocolatebeads were estimated by a color and appearance measure-ment system (Lovibond CAM-System 500 Great Britain)e system was calibrated using the GretagMacbeth minicolor checker model PN50111 to obtain Llowast alowast and blowast CIEvalues e chroma (C) was also calculated according toequation (1) as follows [30]

Chroma(C) alowast

( 11138572

+ blowast

( 11138572

1113872 111387305

(1)

224 Total Phenolic Content (TPC) e TPC of alginatebeads was determined by the Folin-Ciocalteu method withmodifications [4 31] Briefly 05 g of beads was mixed with10ml of 1 wv acetic acid solution homogenized usingULTRA-TURRAX (T25 IKA) at 10000 rpm for 30 sec emixture was finally centrifuged 4000 rpm10min) andsupernatants were collected for further analysis An aliquotof 100 μl of the supernatant was mixed with 100 μl of Folin-Ciocalteu reagent in a 15ml Eppendorf tube and allowed toreact for 2min After that 800 μl of Na2CO3 solution (5wv) was added and the tubes were incubated in a water bathfor 20min at 40degC e absorbance of the samples wasrecorded at 740 nm using appropriate blanks containingformic acid solution Total phenolic content concentration(TPC) was estimated by using a gallic acid calibration curve(10ndash80mgml) e results were expressed as gallic acidequivalents (mg GAEg of beads)

2 Journal of Food Quality

225 Radical Scavenging Activity Determination e anti-oxidant activity of chocolate beads was evaluated by scavengingof DPPHbull A 25μl aliquot of the beadsrsquo supernatant prepared asdescribed previously for TPC analysis was mixed with 925μlfreshly prepared DPPHbull solution (80mM) e mixture wasincubated for 30min at room temperature (25degC) and theabsorbance was measured at 515nm

e radical scavenging activity of the beads was finallyestimated according to [32] and the results are expressed aspercentage of inhibition (I) against blank according toequation (2)

(I) 100 timesA0 minus As( 1113857

A0 (2)

where A0 and As are the absorbances at 515 nm of the blankand sample respectively

226 Sensory Evaluation Sensory evaluation was performedby a panel of 15 experiencedmembers (8 female 7male)e 9-point hedonic scale (1 extremely dislike 5 nor like nordislike and 9 extremely like) was used to evaluate selectedsamples of chocolate beads (control and samples with 6wwMLE) in terms of color taste aroma texture and generalacceptance [33]

227 Statistical Analysis All physicochemical analyses wereperformed in triplicate e statistical analysis was

performed with StatGraphics Centurion XV software bymeans of analysis of variance (ANOVA) Fisherrsquos leastsignificant difference (LSD) test was used to discriminateamong sample means at 95 level of confidence (plt 005)

3 Results and Discussion

31 Chocolate Bead Size Manufacturing parameters (nozzlediameter distance of the nozzle from the gelling solutiontemperature polymer solution feed rate cross-linking agentconcentration) and alginate properties (polymer concen-tration molecular weight) can be modified to alter or op-timize the geometric properties of the beads [34 35]

In Figures 1 and 2(a)ndash2(d) the appearance and geo-metric properties of control and MLE chocolate beads aredemonstrated For presentation reasons in Figure 1 onlyconcentration (0 and 6 ww MLE) and hardening timeextremes (2 and 20min) are depicted e Feret diameterdefined as the maximum caliper of an object varied between430 and 502mm (Figure 2(a)) A gradual decrease of thebeadsrsquo diameter was observed by increasing the MLE con-centration from 0 to 6 ww e diameter of control beadsranged between sim48 and 50mm whereas those at maxi-mum MLE concentration were around 43mm wide esame trend was observed for area and perimeter (Figure 2(b)and 2(c)) that decreased by almost 22 and 12 respectivelywhen MLE concentration increased from 0 to 6 wwSimilar findings have been referred in other studies on

Hardening time 0 ww MLE 6 ww MLE

20 min

2 min

Figure 1 Appearance of chocolate alginate beads as affected by MLE concentration and hardening time

Journal of Food Quality 3

alginate beads with added extracts or phenolic compoundsKannat et al [36] reported that the size of alginate beads wasreduced from 242 to 205mm upon the addition of onionscale extract from 0 up to 6 ww Smaller bead size was alsoobserved for beads with incorporated caffeine [37] It hasbeen also documented that several phenolic compoundshave the ability to lower the surface tension of solutionswhich may explain the observed decrease in size [38]

However increasing the curing time from 2 to 20mindid not result in beads smaller in size (plt 005) e op-posite phenomenon has been referred in other studies Asshown elsewhere the time allowed for gelation in calciumchloride bath had a major effect on bead size but the in-fluence on shape is less intense [39] Long curing timeresulted in smaller beads due to extensive cross-linking thatincreased the rigidity of the beadmatrix In the same study itis also recommended that the total dripping time is limitedto 2ndash3min and curing time between 15ndash20min to avoidexcessive shrinkage and increased polydispersity within thesample Smaller and more spherical beads were obtainedwith prolonged curing time up to 30min [35]

Circularity values equal to 1 indicate geometries of aperfect circle while those approaching 0 correspond toelongated shapes A slight increase in circularity values from093 to 094 was detected by increasing the MLE concen-tration although significant differences compared withcontrol samples were observed only when 6 ww of extractwas added Hence less elongated beads were produced atmaximum MLE concentration

It could be therefore concluded that the glycerol con-tained in the MLE is the main factor governing the size andthe rest geometrical properties of the alginate beads ratherthan the curing time

32 Color Properties Color is considered a key property forfood products as it can affect other important sensorycharacteristics related to consumer acceptance and pur-chasing intention [40 41]

Figure 3(a)ndash3(d) shows the influence of MLE concen-tration and hardening time on the color properties (Llowast alowastblowast) and chroma of alginate beads Llowast alowast and blowast values of allsamples prepared ranged between 307 and 393 81 and132 and 66 and 113 respectively resembling the color ofchocolate bars [42] Peak values for lightness were observedat 4 ww MLE concentration (Llowast 384ndash393) whereasslightly lower values were observed at 6 ww An increaseof redness and yellowness (positive alowast and blowast values) wasalso observed by increasing MLE concentration of the al-ginate solution up to 4 ww but it remained practicallyunaffected at the maximum MLE concentration e sametrend was also observed for chroma as it is a propertygenerated by alowast and blowast values is is due to the pigmentspresent in the MLE that impart a yellowish appearance to itInterestingly the trend observed for the lightness of thebeads as affected by MLE content correlated with that ob-served for TPC (Figure 4) More specifically as TPC initiallydecreased an increase in Llowast values was observed and the

aA aAB aAB

aB

aA

aAaA

aA

bA

aB aBaB

9

11

13

15

17

0 2 4 6

Are

a (m

m2 )

Moringa oleifera leaf extract concentration (ww)

2 min8 min20 min

(a)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaAB

aAB

aB

aA aAB

aBaB

bAaB

aC aC

111213141516

Perim

eter

(mm

)

2 min8 min20 min

(b)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aA

aA

aA aAB

aABaB

bAaA

aBaB

4

5

6

Fere

t dia

met

er (m

m)

2 min8 min20 min

(c)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aA

aAB

aABaAB

aA

aAB

aABaAB

aA aA

aABaB

090091092093094095096

Circ

ular

ity (ndash

)2 min8 min20 min

(d)

Figure 2 Geometric properties of chocolate alginate beads as affected byMLE concentration (0 2 4 and 6 ww) and hardening time (2 8and 20min) Different small letters indicate significant differences among samples of the same concentration while different capital lettersindicate significant differences among samples of the same hardening time at plt 005

4 Journal of Food Quality

abA

aB

aDaC

bA

aB

aC

aB

aA

aB

aD

aC

25

30

35

40

45

0 2 4 6

L (ndash

)

Moringa oleifera leaf extract concentration (ww)

2 min8 min20 min

(a)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aA aA

aB

aB

aA

aB

aC

bC

aA

aB

aC

aC

6

7

8

9

10

11

12

13

14

a (ndash)

2 min8 min20 min

(b)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aB

aB

aA aA

aCaB

aA

aA

aB aB

456789

10111213

b (ndash

)

2 min8 min20 min

(c)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aC

aB

aA

aB

aC bC

aA aA

aB

abB

8

10

12

14

16

18

Chro

ma (

ndash)

2 min8 min20 min

(d)

Figure 3 CIE Llowast alowast and blowast and chroma color properties of chocolate alginate beads as affected byMLE concentration (0 2 4 and 6 ww)and hardening time (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentrationwhile different capital letters indicate significant differences among samples of the same hardening time at plt 005

bBcB

bA

bC

bB

bAaA

aBaB

aA aA

aC

060

080

100

120

140

160

0 2 4 6

TPC

(mg

GA

Eg)

Moringa oleifera leaf extract (ww)

2 min8 min20 min

Figure 4 Total phenolic content (TPC) of chocolate alginate beads as affected by MLE concentration (0 2 4 and 6 ww) and hardeningtime (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentration while differentcapital letters indicate significant differences among samples of the same hardening time at plt 005

Journal of Food Quality 5

subsequent increase of phenolic compounds (6 ww MLE)corresponded to decreased Llowast is was also observed inother studies [43] However the TPC decrease observedupon increasing of hardening time did not alter the Llowast valuesas expected erefore a more detailed study is needed tofully elucidate the effect of MLE on lightness as other typesof compounds such as melanoidins may contribute to theoccurring color changes Melanoidins are high-molecular-weight dark brown derivatives formed during the roasting ofcocoa beans due to polyphenol degradation through theMaillard reaction [44]

For the vast majority of samples the time allowed forcross-linking in the ionic solution did not significantly affectthe color properties of the samples (pgt 005)

33 Total Phenolic Content (TPC) Process parameters thatmay affect polyphenol loading of alginate beads apart fromextract concentration include sodium alginate concentra-tion calcium chloride concentration and exposure time[20]

In Figure 4 the effect of extract concentration andhardening time on TPC content of alginate beads is depictedIn total the phenolic content of the samples varied between088 and 138mg GAEg of beads Similar contents havebeen reported in other studies involving the encapsulation ofherbal extract in alginate beads [45] Both parametersstudied (MLE concentration and hardening time) had aprofound effect on TPC values Although an increase inphenolic content would be expected by increasing the extractconcentration in the alginate solution this was not observedin our case A gradual decrease of TPC was observed uponincrease of the extract added up to 4 ww after which itwas finally increased is trend was observed in all casesregardless of the hardening time used e above phe-nomenon could be induced by the presence of high amountsof glycerol in the beads which is the main component ofDES used for the preparation of the Moringa extractGlycerol is a known plasticizer with low molecular weight

Glycerol concentration above a critical value which dependson the molecular weight of alginates may induce chemicalinteractions that modify the mechanical morphological andbarrier properties of alginate polymer films [46 47] esmall size of glycerol facilitates its penetration between al-ginate hydrogen bonds resulting in reduced intermolecularforces that increase the mobility of the polymer chains As aconsequence less compact polymer matrices are formedwith increased elasticity [48] As shown by Ion [49] theincreased firmness in alginate-chitosan complexes wascaused by enhanced intermolecular interactions of car-boxylate groups found in alginates and the amine groups ofchitosanis favored the entrapment of polyphenols duringthe ionotropic gelation as evidenced by higher encapsula-tion efficiency rates compared with control beads that didnot contain chitosan

Hardening time also had a considerable effect on theTPC of the beads As seen in Figure 4 significantly lowerTPCs were observed after 20min of immersion in the cal-cium solution in all cases of samples compared with beadsexposed for 2min is 10-fold time increase resulted inTPC values decreased by sim16 on average Hence theminimum and maximum phenolic content were observed insamples containing 2 ww MLE treated for 20min andsamples with 6 ww extract treated in Ca2+ solution for2min

As previously reported calcium chloride exposure timemay decrease the loading efficiency of several compoundsIndeed prolonged exposure may cause a shift of Ca2+ boundwithin the alginate matrix or excessive release of polyphenols[20]

34 Antioxidant Activity e DPPHbull radical scavengingactivity of MLE chocolate beads prepared by varying extractconcentration and CaCl2 immersion time is shown inFigure 5 As can be seen the effect of MLE concentration onthe antioxidant activity of the beads is related to the curingtime used for sample preparation For beads allowed toharden for 2min percentage inhibition (I) values slightlyincreased from sim98 to 131 when increasing MLE con-centration although no significant differences were foundamong samples (pgt 005) On the contrary samples treatedfor 8 and 20min presented significantly enhanced antioxi-dant activity when 6 ww of MLE was added comparedwith control samples (plt 005)

Our results also show that the antioxidant activity of thebeads was unaffected by different time intervals used for thehardening of the beads for samples with the same extractconcentration (pgt 005)

Interestingly DPPH inhibition values did not correlatewith corresponding phenolic content shown previously inFigure 4 More specifically despite the reduction of TPCobserved as hardening time increased from 2 to 20minDPPHbull inhibition percentages were similar among sampleswith the same MLE concentration In addition althoughsamples prepared at 2min had higher TPC still they wereequally potent with the rest of the samples in terms of radicalscavenging (pgt 005)

aA aA aA

aB

aA aAaA

aB

aA

aA

aA

aB

6

8

10

12

14

16

0 2 4 6

Inhi

bitio

n (

)

Moringa oleifera extract concentration (ww)

2 min8 min20 min

Figure 5 Radical scavenging capacity (I) of chocolate alginatebeads as affected by MLE concentration (0 2 4 and 6 ww) andhardening time (2 8 and 20min) Different small letters indicatesignificant differences among samples of the same concentrationwhile different capital letters indicate significant differences amongsamples of the same hardening time at plt 005

6 Journal of Food Quality

A possible explanation would be that the loss of poly-phenols caused by prolonged hardening of the beads thatwash off from the beadsrsquo matrix was not extensive enough toaffect their radical scavenging capacity drastically

On the other hand as previously referred melanoidinsthat result from polyphenol degradation are considered thepredominant contributors of the antioxidant activity ofcocoa beans [44] e researchers of this study found thateven though TPC of roasted cocoa beans was significantlylower than that of the raw material the antioxidant activitywas the same for both samples Hence the reduction in TPCmay have not altered the antioxidant potential of the alginatebeads detrimentally

35 Sensory Evaluation Control samples and samplescontaining 6wwMLE were selected for sensory evaluationas the later presented the highest TPC and DPPH valuesIn Table 1 the scores of different sensory attributes aredisplayed In general all samples were well accepted bypanelists as values for general acceptance color tastearoma and texture ranged between 58 and 76 e ad-dition of MLE did not impart any unfavorable attributesto the samples as evidenced by similar sensory scores Nosignificant differences were detected among samplesprepared with different curing times in terms of colortaste aroma and general acceptance (plt 005) Findingsfor color are in line with those demonstrated in Figure 3showing that since curing time did not alter the colorproperties of the beads the panelists showed the sameacceptance On the other hand curing time extremes (2and 20min) negatively affected the acceptance of textureas slightly lower values were obtained for these samplesis was observed for both types of samples control andsamples with added MLE It could be therefore concludedthat chocolate beads containing 6 ww MLE cured for8min represent the sample with well-accepted sensoryattributes and most pleasant texture

4 Conclusions

Moringa oleifera leaf extract (MLE) prepared by a ldquogreenrdquoextraction technology rich in phenolic ingredients wasencapsulated in chocolate-flavored alginate beads e ap-pearance of the beads including geometric and colorproperties was affected by the amount of extract

incorporated e higher the amount of MLE added thehigher the redness yellowness and chroma of the beadswhich also became less elliptical in shape e amount ofMLE added as well as the hardening time was also critical interms of the phenolic compounds found in the final productAs a result a minimum TPC concentration of 084mg GAEg beads was established for beads prepared with 2 wwMLE allowed 20min in CaCl2 to harden However theradical scavenging activity was only concentration-relatedand a minimum 6 ww of MLE is required to enhance itsinhibitory effect e beads prepared with maximum MLEconcentration cured for 8min had the most favorable tex-ture so they can be added in food dessert products to en-hance their antioxidant potential

Data Availability

e data used to support the findings of this study are in-cluded within the article

Conflicts of Interest

e authors declare no conflicts of interest

Acknowledgments

is research has been cofinanced by the European Unionand Greek national funds through the Operational ProgramCompetitiveness Entrepreneurship and Innovation underthe call RESEARCH - CREATE - INNOVATE (project codeT1EDK-05677)

References

[1] A Rashidinejad and S M Jafari Handbook of Food Nano-technology S M Jafari Ed Academic Press Cambridge MAUSA pp 279ndash344 2020

[2] V Nedovic A Kalusevic V Manojlovic S Levic andB Bugarski ldquoAn overview of encapsulation technologies forfood applicationsrdquo Procedia Food Science vol 1 pp 1806ndash1815 2011

[3] S Castro Coelho B Nogueiro Estevinho and F RochaldquoEncapsulation in food industry with emerging electro-hydrodynamic techniques electrospinning and electro-sprayingmdasha reviewrdquo Food Chemistry vol 339 Article ID127850 2021

[4] A Lakka S Grigorakis O Kaltsa et al ldquoe effect ofultrasonication pretreatment on the production of

Table 1 Sensory evaluation scores of chocolate alginate beads (control and 6 ww MLE) prepared with different hardening times

Color Taste Aroma Texture General acceptanceControl2min 707aplusmn 088 607aplusmn 080 680aplusmn 086 653abplusmn 064 680aplusmn 0568min 713aplusmn 052 620aplusmn 077 653aplusmn 099 740cplusmn 051 700aplusmn 06520min 707aplusmn 070 627aplusmn 070 673aplusmn 046 620aplusmn 077 687aplusmn 0646 MLE2min 740aplusmn 051 627aplusmn 080 647aplusmn 074 687 bplusmn 035 707aplusmn 0468min 700aplusmn 065 580aplusmn 086 660aplusmn 099 767cplusmn 049 720aplusmn 04120min 673aplusmn 059 600aplusmn 085 633aplusmn 082 653abplusmn 052 720aplusmn 056Within the same column values followed by different letters are significantly different (plt 005)

Journal of Food Quality 7

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

alginate beads with added extracts or phenolic compoundsKannat et al [36] reported that the size of alginate beads wasreduced from 242 to 205mm upon the addition of onionscale extract from 0 up to 6 ww Smaller bead size was alsoobserved for beads with incorporated caffeine [37] It hasbeen also documented that several phenolic compoundshave the ability to lower the surface tension of solutionswhich may explain the observed decrease in size [38]

However increasing the curing time from 2 to 20mindid not result in beads smaller in size (plt 005) e op-posite phenomenon has been referred in other studies Asshown elsewhere the time allowed for gelation in calciumchloride bath had a major effect on bead size but the in-fluence on shape is less intense [39] Long curing timeresulted in smaller beads due to extensive cross-linking thatincreased the rigidity of the beadmatrix In the same study itis also recommended that the total dripping time is limitedto 2ndash3min and curing time between 15ndash20min to avoidexcessive shrinkage and increased polydispersity within thesample Smaller and more spherical beads were obtainedwith prolonged curing time up to 30min [35]

Circularity values equal to 1 indicate geometries of aperfect circle while those approaching 0 correspond toelongated shapes A slight increase in circularity values from093 to 094 was detected by increasing the MLE concen-tration although significant differences compared withcontrol samples were observed only when 6 ww of extractwas added Hence less elongated beads were produced atmaximum MLE concentration

It could be therefore concluded that the glycerol con-tained in the MLE is the main factor governing the size andthe rest geometrical properties of the alginate beads ratherthan the curing time

32 Color Properties Color is considered a key property forfood products as it can affect other important sensorycharacteristics related to consumer acceptance and pur-chasing intention [40 41]

Figure 3(a)ndash3(d) shows the influence of MLE concen-tration and hardening time on the color properties (Llowast alowastblowast) and chroma of alginate beads Llowast alowast and blowast values of allsamples prepared ranged between 307 and 393 81 and132 and 66 and 113 respectively resembling the color ofchocolate bars [42] Peak values for lightness were observedat 4 ww MLE concentration (Llowast 384ndash393) whereasslightly lower values were observed at 6 ww An increaseof redness and yellowness (positive alowast and blowast values) wasalso observed by increasing MLE concentration of the al-ginate solution up to 4 ww but it remained practicallyunaffected at the maximum MLE concentration e sametrend was also observed for chroma as it is a propertygenerated by alowast and blowast values is is due to the pigmentspresent in the MLE that impart a yellowish appearance to itInterestingly the trend observed for the lightness of thebeads as affected by MLE content correlated with that ob-served for TPC (Figure 4) More specifically as TPC initiallydecreased an increase in Llowast values was observed and the

aA aAB aAB

aB

aA

aAaA

aA

bA

aB aBaB

9

11

13

15

17

0 2 4 6

Are

a (m

m2 )

Moringa oleifera leaf extract concentration (ww)

2 min8 min20 min

(a)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaAB

aAB

aB

aA aAB

aBaB

bAaB

aC aC

111213141516

Perim

eter

(mm

)

2 min8 min20 min

(b)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aA

aA

aA aAB

aABaB

bAaA

aBaB

4

5

6

Fere

t dia

met

er (m

m)

2 min8 min20 min

(c)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aA

aAB

aABaAB

aA

aAB

aABaAB

aA aA

aABaB

090091092093094095096

Circ

ular

ity (ndash

)2 min8 min20 min

(d)

Figure 2 Geometric properties of chocolate alginate beads as affected byMLE concentration (0 2 4 and 6 ww) and hardening time (2 8and 20min) Different small letters indicate significant differences among samples of the same concentration while different capital lettersindicate significant differences among samples of the same hardening time at plt 005

4 Journal of Food Quality

abA

aB

aDaC

bA

aB

aC

aB

aA

aB

aD

aC

25

30

35

40

45

0 2 4 6

L (ndash

)

Moringa oleifera leaf extract concentration (ww)

2 min8 min20 min

(a)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aA aA

aB

aB

aA

aB

aC

bC

aA

aB

aC

aC

6

7

8

9

10

11

12

13

14

a (ndash)

2 min8 min20 min

(b)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aB

aB

aA aA

aCaB

aA

aA

aB aB

456789

10111213

b (ndash

)

2 min8 min20 min

(c)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aC

aB

aA

aB

aC bC

aA aA

aB

abB

8

10

12

14

16

18

Chro

ma (

ndash)

2 min8 min20 min

(d)

Figure 3 CIE Llowast alowast and blowast and chroma color properties of chocolate alginate beads as affected byMLE concentration (0 2 4 and 6 ww)and hardening time (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentrationwhile different capital letters indicate significant differences among samples of the same hardening time at plt 005

bBcB

bA

bC

bB

bAaA

aBaB

aA aA

aC

060

080

100

120

140

160

0 2 4 6

TPC

(mg

GA

Eg)

Moringa oleifera leaf extract (ww)

2 min8 min20 min

Figure 4 Total phenolic content (TPC) of chocolate alginate beads as affected by MLE concentration (0 2 4 and 6 ww) and hardeningtime (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentration while differentcapital letters indicate significant differences among samples of the same hardening time at plt 005

Journal of Food Quality 5

subsequent increase of phenolic compounds (6 ww MLE)corresponded to decreased Llowast is was also observed inother studies [43] However the TPC decrease observedupon increasing of hardening time did not alter the Llowast valuesas expected erefore a more detailed study is needed tofully elucidate the effect of MLE on lightness as other typesof compounds such as melanoidins may contribute to theoccurring color changes Melanoidins are high-molecular-weight dark brown derivatives formed during the roasting ofcocoa beans due to polyphenol degradation through theMaillard reaction [44]

For the vast majority of samples the time allowed forcross-linking in the ionic solution did not significantly affectthe color properties of the samples (pgt 005)

33 Total Phenolic Content (TPC) Process parameters thatmay affect polyphenol loading of alginate beads apart fromextract concentration include sodium alginate concentra-tion calcium chloride concentration and exposure time[20]

In Figure 4 the effect of extract concentration andhardening time on TPC content of alginate beads is depictedIn total the phenolic content of the samples varied between088 and 138mg GAEg of beads Similar contents havebeen reported in other studies involving the encapsulation ofherbal extract in alginate beads [45] Both parametersstudied (MLE concentration and hardening time) had aprofound effect on TPC values Although an increase inphenolic content would be expected by increasing the extractconcentration in the alginate solution this was not observedin our case A gradual decrease of TPC was observed uponincrease of the extract added up to 4 ww after which itwas finally increased is trend was observed in all casesregardless of the hardening time used e above phe-nomenon could be induced by the presence of high amountsof glycerol in the beads which is the main component ofDES used for the preparation of the Moringa extractGlycerol is a known plasticizer with low molecular weight

Glycerol concentration above a critical value which dependson the molecular weight of alginates may induce chemicalinteractions that modify the mechanical morphological andbarrier properties of alginate polymer films [46 47] esmall size of glycerol facilitates its penetration between al-ginate hydrogen bonds resulting in reduced intermolecularforces that increase the mobility of the polymer chains As aconsequence less compact polymer matrices are formedwith increased elasticity [48] As shown by Ion [49] theincreased firmness in alginate-chitosan complexes wascaused by enhanced intermolecular interactions of car-boxylate groups found in alginates and the amine groups ofchitosanis favored the entrapment of polyphenols duringthe ionotropic gelation as evidenced by higher encapsula-tion efficiency rates compared with control beads that didnot contain chitosan

Hardening time also had a considerable effect on theTPC of the beads As seen in Figure 4 significantly lowerTPCs were observed after 20min of immersion in the cal-cium solution in all cases of samples compared with beadsexposed for 2min is 10-fold time increase resulted inTPC values decreased by sim16 on average Hence theminimum and maximum phenolic content were observed insamples containing 2 ww MLE treated for 20min andsamples with 6 ww extract treated in Ca2+ solution for2min

As previously reported calcium chloride exposure timemay decrease the loading efficiency of several compoundsIndeed prolonged exposure may cause a shift of Ca2+ boundwithin the alginate matrix or excessive release of polyphenols[20]

34 Antioxidant Activity e DPPHbull radical scavengingactivity of MLE chocolate beads prepared by varying extractconcentration and CaCl2 immersion time is shown inFigure 5 As can be seen the effect of MLE concentration onthe antioxidant activity of the beads is related to the curingtime used for sample preparation For beads allowed toharden for 2min percentage inhibition (I) values slightlyincreased from sim98 to 131 when increasing MLE con-centration although no significant differences were foundamong samples (pgt 005) On the contrary samples treatedfor 8 and 20min presented significantly enhanced antioxi-dant activity when 6 ww of MLE was added comparedwith control samples (plt 005)

Our results also show that the antioxidant activity of thebeads was unaffected by different time intervals used for thehardening of the beads for samples with the same extractconcentration (pgt 005)

Interestingly DPPH inhibition values did not correlatewith corresponding phenolic content shown previously inFigure 4 More specifically despite the reduction of TPCobserved as hardening time increased from 2 to 20minDPPHbull inhibition percentages were similar among sampleswith the same MLE concentration In addition althoughsamples prepared at 2min had higher TPC still they wereequally potent with the rest of the samples in terms of radicalscavenging (pgt 005)

aA aA aA

aB

aA aAaA

aB

aA

aA

aA

aB

6

8

10

12

14

16

0 2 4 6

Inhi

bitio

n (

)

Moringa oleifera extract concentration (ww)

2 min8 min20 min

Figure 5 Radical scavenging capacity (I) of chocolate alginatebeads as affected by MLE concentration (0 2 4 and 6 ww) andhardening time (2 8 and 20min) Different small letters indicatesignificant differences among samples of the same concentrationwhile different capital letters indicate significant differences amongsamples of the same hardening time at plt 005

6 Journal of Food Quality

A possible explanation would be that the loss of poly-phenols caused by prolonged hardening of the beads thatwash off from the beadsrsquo matrix was not extensive enough toaffect their radical scavenging capacity drastically

On the other hand as previously referred melanoidinsthat result from polyphenol degradation are considered thepredominant contributors of the antioxidant activity ofcocoa beans [44] e researchers of this study found thateven though TPC of roasted cocoa beans was significantlylower than that of the raw material the antioxidant activitywas the same for both samples Hence the reduction in TPCmay have not altered the antioxidant potential of the alginatebeads detrimentally

35 Sensory Evaluation Control samples and samplescontaining 6wwMLE were selected for sensory evaluationas the later presented the highest TPC and DPPH valuesIn Table 1 the scores of different sensory attributes aredisplayed In general all samples were well accepted bypanelists as values for general acceptance color tastearoma and texture ranged between 58 and 76 e ad-dition of MLE did not impart any unfavorable attributesto the samples as evidenced by similar sensory scores Nosignificant differences were detected among samplesprepared with different curing times in terms of colortaste aroma and general acceptance (plt 005) Findingsfor color are in line with those demonstrated in Figure 3showing that since curing time did not alter the colorproperties of the beads the panelists showed the sameacceptance On the other hand curing time extremes (2and 20min) negatively affected the acceptance of textureas slightly lower values were obtained for these samplesis was observed for both types of samples control andsamples with added MLE It could be therefore concludedthat chocolate beads containing 6 ww MLE cured for8min represent the sample with well-accepted sensoryattributes and most pleasant texture

4 Conclusions

Moringa oleifera leaf extract (MLE) prepared by a ldquogreenrdquoextraction technology rich in phenolic ingredients wasencapsulated in chocolate-flavored alginate beads e ap-pearance of the beads including geometric and colorproperties was affected by the amount of extract

incorporated e higher the amount of MLE added thehigher the redness yellowness and chroma of the beadswhich also became less elliptical in shape e amount ofMLE added as well as the hardening time was also critical interms of the phenolic compounds found in the final productAs a result a minimum TPC concentration of 084mg GAEg beads was established for beads prepared with 2 wwMLE allowed 20min in CaCl2 to harden However theradical scavenging activity was only concentration-relatedand a minimum 6 ww of MLE is required to enhance itsinhibitory effect e beads prepared with maximum MLEconcentration cured for 8min had the most favorable tex-ture so they can be added in food dessert products to en-hance their antioxidant potential

Data Availability

e data used to support the findings of this study are in-cluded within the article

Conflicts of Interest

e authors declare no conflicts of interest

Acknowledgments

is research has been cofinanced by the European Unionand Greek national funds through the Operational ProgramCompetitiveness Entrepreneurship and Innovation underthe call RESEARCH - CREATE - INNOVATE (project codeT1EDK-05677)

References

[1] A Rashidinejad and S M Jafari Handbook of Food Nano-technology S M Jafari Ed Academic Press Cambridge MAUSA pp 279ndash344 2020

[2] V Nedovic A Kalusevic V Manojlovic S Levic andB Bugarski ldquoAn overview of encapsulation technologies forfood applicationsrdquo Procedia Food Science vol 1 pp 1806ndash1815 2011

[3] S Castro Coelho B Nogueiro Estevinho and F RochaldquoEncapsulation in food industry with emerging electro-hydrodynamic techniques electrospinning and electro-sprayingmdasha reviewrdquo Food Chemistry vol 339 Article ID127850 2021

[4] A Lakka S Grigorakis O Kaltsa et al ldquoe effect ofultrasonication pretreatment on the production of

Table 1 Sensory evaluation scores of chocolate alginate beads (control and 6 ww MLE) prepared with different hardening times

Color Taste Aroma Texture General acceptanceControl2min 707aplusmn 088 607aplusmn 080 680aplusmn 086 653abplusmn 064 680aplusmn 0568min 713aplusmn 052 620aplusmn 077 653aplusmn 099 740cplusmn 051 700aplusmn 06520min 707aplusmn 070 627aplusmn 070 673aplusmn 046 620aplusmn 077 687aplusmn 0646 MLE2min 740aplusmn 051 627aplusmn 080 647aplusmn 074 687 bplusmn 035 707aplusmn 0468min 700aplusmn 065 580aplusmn 086 660aplusmn 099 767cplusmn 049 720aplusmn 04120min 673aplusmn 059 600aplusmn 085 633aplusmn 082 653abplusmn 052 720aplusmn 056Within the same column values followed by different letters are significantly different (plt 005)

Journal of Food Quality 7

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

abA

aB

aDaC

bA

aB

aC

aB

aA

aB

aD

aC

25

30

35

40

45

0 2 4 6

L (ndash

)

Moringa oleifera leaf extract concentration (ww)

2 min8 min20 min

(a)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aA aA

aB

aB

aA

aB

aC

bC

aA

aB

aC

aC

6

7

8

9

10

11

12

13

14

a (ndash)

2 min8 min20 min

(b)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aB

aB

aA aA

aCaB

aA

aA

aB aB

456789

10111213

b (ndash

)

2 min8 min20 min

(c)

0 2 4 6Moringa oleifera leaf extract concentration (ww)

aAaA

aC

aB

aA

aB

aC bC

aA aA

aB

abB

8

10

12

14

16

18

Chro

ma (

ndash)

2 min8 min20 min

(d)

Figure 3 CIE Llowast alowast and blowast and chroma color properties of chocolate alginate beads as affected byMLE concentration (0 2 4 and 6 ww)and hardening time (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentrationwhile different capital letters indicate significant differences among samples of the same hardening time at plt 005

bBcB

bA

bC

bB

bAaA

aBaB

aA aA

aC

060

080

100

120

140

160

0 2 4 6

TPC

(mg

GA

Eg)

Moringa oleifera leaf extract (ww)

2 min8 min20 min

Figure 4 Total phenolic content (TPC) of chocolate alginate beads as affected by MLE concentration (0 2 4 and 6 ww) and hardeningtime (2 8 and 20min) Different small letters indicate significant differences among samples of the same concentration while differentcapital letters indicate significant differences among samples of the same hardening time at plt 005

Journal of Food Quality 5

subsequent increase of phenolic compounds (6 ww MLE)corresponded to decreased Llowast is was also observed inother studies [43] However the TPC decrease observedupon increasing of hardening time did not alter the Llowast valuesas expected erefore a more detailed study is needed tofully elucidate the effect of MLE on lightness as other typesof compounds such as melanoidins may contribute to theoccurring color changes Melanoidins are high-molecular-weight dark brown derivatives formed during the roasting ofcocoa beans due to polyphenol degradation through theMaillard reaction [44]

For the vast majority of samples the time allowed forcross-linking in the ionic solution did not significantly affectthe color properties of the samples (pgt 005)

33 Total Phenolic Content (TPC) Process parameters thatmay affect polyphenol loading of alginate beads apart fromextract concentration include sodium alginate concentra-tion calcium chloride concentration and exposure time[20]

In Figure 4 the effect of extract concentration andhardening time on TPC content of alginate beads is depictedIn total the phenolic content of the samples varied between088 and 138mg GAEg of beads Similar contents havebeen reported in other studies involving the encapsulation ofherbal extract in alginate beads [45] Both parametersstudied (MLE concentration and hardening time) had aprofound effect on TPC values Although an increase inphenolic content would be expected by increasing the extractconcentration in the alginate solution this was not observedin our case A gradual decrease of TPC was observed uponincrease of the extract added up to 4 ww after which itwas finally increased is trend was observed in all casesregardless of the hardening time used e above phe-nomenon could be induced by the presence of high amountsof glycerol in the beads which is the main component ofDES used for the preparation of the Moringa extractGlycerol is a known plasticizer with low molecular weight

Glycerol concentration above a critical value which dependson the molecular weight of alginates may induce chemicalinteractions that modify the mechanical morphological andbarrier properties of alginate polymer films [46 47] esmall size of glycerol facilitates its penetration between al-ginate hydrogen bonds resulting in reduced intermolecularforces that increase the mobility of the polymer chains As aconsequence less compact polymer matrices are formedwith increased elasticity [48] As shown by Ion [49] theincreased firmness in alginate-chitosan complexes wascaused by enhanced intermolecular interactions of car-boxylate groups found in alginates and the amine groups ofchitosanis favored the entrapment of polyphenols duringthe ionotropic gelation as evidenced by higher encapsula-tion efficiency rates compared with control beads that didnot contain chitosan

Hardening time also had a considerable effect on theTPC of the beads As seen in Figure 4 significantly lowerTPCs were observed after 20min of immersion in the cal-cium solution in all cases of samples compared with beadsexposed for 2min is 10-fold time increase resulted inTPC values decreased by sim16 on average Hence theminimum and maximum phenolic content were observed insamples containing 2 ww MLE treated for 20min andsamples with 6 ww extract treated in Ca2+ solution for2min

As previously reported calcium chloride exposure timemay decrease the loading efficiency of several compoundsIndeed prolonged exposure may cause a shift of Ca2+ boundwithin the alginate matrix or excessive release of polyphenols[20]

34 Antioxidant Activity e DPPHbull radical scavengingactivity of MLE chocolate beads prepared by varying extractconcentration and CaCl2 immersion time is shown inFigure 5 As can be seen the effect of MLE concentration onthe antioxidant activity of the beads is related to the curingtime used for sample preparation For beads allowed toharden for 2min percentage inhibition (I) values slightlyincreased from sim98 to 131 when increasing MLE con-centration although no significant differences were foundamong samples (pgt 005) On the contrary samples treatedfor 8 and 20min presented significantly enhanced antioxi-dant activity when 6 ww of MLE was added comparedwith control samples (plt 005)

Our results also show that the antioxidant activity of thebeads was unaffected by different time intervals used for thehardening of the beads for samples with the same extractconcentration (pgt 005)

Interestingly DPPH inhibition values did not correlatewith corresponding phenolic content shown previously inFigure 4 More specifically despite the reduction of TPCobserved as hardening time increased from 2 to 20minDPPHbull inhibition percentages were similar among sampleswith the same MLE concentration In addition althoughsamples prepared at 2min had higher TPC still they wereequally potent with the rest of the samples in terms of radicalscavenging (pgt 005)

aA aA aA

aB

aA aAaA

aB

aA

aA

aA

aB

6

8

10

12

14

16

0 2 4 6

Inhi

bitio

n (

)

Moringa oleifera extract concentration (ww)

2 min8 min20 min

Figure 5 Radical scavenging capacity (I) of chocolate alginatebeads as affected by MLE concentration (0 2 4 and 6 ww) andhardening time (2 8 and 20min) Different small letters indicatesignificant differences among samples of the same concentrationwhile different capital letters indicate significant differences amongsamples of the same hardening time at plt 005

6 Journal of Food Quality

A possible explanation would be that the loss of poly-phenols caused by prolonged hardening of the beads thatwash off from the beadsrsquo matrix was not extensive enough toaffect their radical scavenging capacity drastically

On the other hand as previously referred melanoidinsthat result from polyphenol degradation are considered thepredominant contributors of the antioxidant activity ofcocoa beans [44] e researchers of this study found thateven though TPC of roasted cocoa beans was significantlylower than that of the raw material the antioxidant activitywas the same for both samples Hence the reduction in TPCmay have not altered the antioxidant potential of the alginatebeads detrimentally

35 Sensory Evaluation Control samples and samplescontaining 6wwMLE were selected for sensory evaluationas the later presented the highest TPC and DPPH valuesIn Table 1 the scores of different sensory attributes aredisplayed In general all samples were well accepted bypanelists as values for general acceptance color tastearoma and texture ranged between 58 and 76 e ad-dition of MLE did not impart any unfavorable attributesto the samples as evidenced by similar sensory scores Nosignificant differences were detected among samplesprepared with different curing times in terms of colortaste aroma and general acceptance (plt 005) Findingsfor color are in line with those demonstrated in Figure 3showing that since curing time did not alter the colorproperties of the beads the panelists showed the sameacceptance On the other hand curing time extremes (2and 20min) negatively affected the acceptance of textureas slightly lower values were obtained for these samplesis was observed for both types of samples control andsamples with added MLE It could be therefore concludedthat chocolate beads containing 6 ww MLE cured for8min represent the sample with well-accepted sensoryattributes and most pleasant texture

4 Conclusions

Moringa oleifera leaf extract (MLE) prepared by a ldquogreenrdquoextraction technology rich in phenolic ingredients wasencapsulated in chocolate-flavored alginate beads e ap-pearance of the beads including geometric and colorproperties was affected by the amount of extract

incorporated e higher the amount of MLE added thehigher the redness yellowness and chroma of the beadswhich also became less elliptical in shape e amount ofMLE added as well as the hardening time was also critical interms of the phenolic compounds found in the final productAs a result a minimum TPC concentration of 084mg GAEg beads was established for beads prepared with 2 wwMLE allowed 20min in CaCl2 to harden However theradical scavenging activity was only concentration-relatedand a minimum 6 ww of MLE is required to enhance itsinhibitory effect e beads prepared with maximum MLEconcentration cured for 8min had the most favorable tex-ture so they can be added in food dessert products to en-hance their antioxidant potential

Data Availability

e data used to support the findings of this study are in-cluded within the article

Conflicts of Interest

e authors declare no conflicts of interest

Acknowledgments

is research has been cofinanced by the European Unionand Greek national funds through the Operational ProgramCompetitiveness Entrepreneurship and Innovation underthe call RESEARCH - CREATE - INNOVATE (project codeT1EDK-05677)

References

[1] A Rashidinejad and S M Jafari Handbook of Food Nano-technology S M Jafari Ed Academic Press Cambridge MAUSA pp 279ndash344 2020

[2] V Nedovic A Kalusevic V Manojlovic S Levic andB Bugarski ldquoAn overview of encapsulation technologies forfood applicationsrdquo Procedia Food Science vol 1 pp 1806ndash1815 2011

[3] S Castro Coelho B Nogueiro Estevinho and F RochaldquoEncapsulation in food industry with emerging electro-hydrodynamic techniques electrospinning and electro-sprayingmdasha reviewrdquo Food Chemistry vol 339 Article ID127850 2021

[4] A Lakka S Grigorakis O Kaltsa et al ldquoe effect ofultrasonication pretreatment on the production of

Table 1 Sensory evaluation scores of chocolate alginate beads (control and 6 ww MLE) prepared with different hardening times

Color Taste Aroma Texture General acceptanceControl2min 707aplusmn 088 607aplusmn 080 680aplusmn 086 653abplusmn 064 680aplusmn 0568min 713aplusmn 052 620aplusmn 077 653aplusmn 099 740cplusmn 051 700aplusmn 06520min 707aplusmn 070 627aplusmn 070 673aplusmn 046 620aplusmn 077 687aplusmn 0646 MLE2min 740aplusmn 051 627aplusmn 080 647aplusmn 074 687 bplusmn 035 707aplusmn 0468min 700aplusmn 065 580aplusmn 086 660aplusmn 099 767cplusmn 049 720aplusmn 04120min 673aplusmn 059 600aplusmn 085 633aplusmn 082 653abplusmn 052 720aplusmn 056Within the same column values followed by different letters are significantly different (plt 005)

Journal of Food Quality 7

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

subsequent increase of phenolic compounds (6 ww MLE)corresponded to decreased Llowast is was also observed inother studies [43] However the TPC decrease observedupon increasing of hardening time did not alter the Llowast valuesas expected erefore a more detailed study is needed tofully elucidate the effect of MLE on lightness as other typesof compounds such as melanoidins may contribute to theoccurring color changes Melanoidins are high-molecular-weight dark brown derivatives formed during the roasting ofcocoa beans due to polyphenol degradation through theMaillard reaction [44]

For the vast majority of samples the time allowed forcross-linking in the ionic solution did not significantly affectthe color properties of the samples (pgt 005)

33 Total Phenolic Content (TPC) Process parameters thatmay affect polyphenol loading of alginate beads apart fromextract concentration include sodium alginate concentra-tion calcium chloride concentration and exposure time[20]

In Figure 4 the effect of extract concentration andhardening time on TPC content of alginate beads is depictedIn total the phenolic content of the samples varied between088 and 138mg GAEg of beads Similar contents havebeen reported in other studies involving the encapsulation ofherbal extract in alginate beads [45] Both parametersstudied (MLE concentration and hardening time) had aprofound effect on TPC values Although an increase inphenolic content would be expected by increasing the extractconcentration in the alginate solution this was not observedin our case A gradual decrease of TPC was observed uponincrease of the extract added up to 4 ww after which itwas finally increased is trend was observed in all casesregardless of the hardening time used e above phe-nomenon could be induced by the presence of high amountsof glycerol in the beads which is the main component ofDES used for the preparation of the Moringa extractGlycerol is a known plasticizer with low molecular weight

Glycerol concentration above a critical value which dependson the molecular weight of alginates may induce chemicalinteractions that modify the mechanical morphological andbarrier properties of alginate polymer films [46 47] esmall size of glycerol facilitates its penetration between al-ginate hydrogen bonds resulting in reduced intermolecularforces that increase the mobility of the polymer chains As aconsequence less compact polymer matrices are formedwith increased elasticity [48] As shown by Ion [49] theincreased firmness in alginate-chitosan complexes wascaused by enhanced intermolecular interactions of car-boxylate groups found in alginates and the amine groups ofchitosanis favored the entrapment of polyphenols duringthe ionotropic gelation as evidenced by higher encapsula-tion efficiency rates compared with control beads that didnot contain chitosan

Hardening time also had a considerable effect on theTPC of the beads As seen in Figure 4 significantly lowerTPCs were observed after 20min of immersion in the cal-cium solution in all cases of samples compared with beadsexposed for 2min is 10-fold time increase resulted inTPC values decreased by sim16 on average Hence theminimum and maximum phenolic content were observed insamples containing 2 ww MLE treated for 20min andsamples with 6 ww extract treated in Ca2+ solution for2min

As previously reported calcium chloride exposure timemay decrease the loading efficiency of several compoundsIndeed prolonged exposure may cause a shift of Ca2+ boundwithin the alginate matrix or excessive release of polyphenols[20]

34 Antioxidant Activity e DPPHbull radical scavengingactivity of MLE chocolate beads prepared by varying extractconcentration and CaCl2 immersion time is shown inFigure 5 As can be seen the effect of MLE concentration onthe antioxidant activity of the beads is related to the curingtime used for sample preparation For beads allowed toharden for 2min percentage inhibition (I) values slightlyincreased from sim98 to 131 when increasing MLE con-centration although no significant differences were foundamong samples (pgt 005) On the contrary samples treatedfor 8 and 20min presented significantly enhanced antioxi-dant activity when 6 ww of MLE was added comparedwith control samples (plt 005)

Our results also show that the antioxidant activity of thebeads was unaffected by different time intervals used for thehardening of the beads for samples with the same extractconcentration (pgt 005)

Interestingly DPPH inhibition values did not correlatewith corresponding phenolic content shown previously inFigure 4 More specifically despite the reduction of TPCobserved as hardening time increased from 2 to 20minDPPHbull inhibition percentages were similar among sampleswith the same MLE concentration In addition althoughsamples prepared at 2min had higher TPC still they wereequally potent with the rest of the samples in terms of radicalscavenging (pgt 005)

aA aA aA

aB

aA aAaA

aB

aA

aA

aA

aB

6

8

10

12

14

16

0 2 4 6

Inhi

bitio

n (

)

Moringa oleifera extract concentration (ww)

2 min8 min20 min

Figure 5 Radical scavenging capacity (I) of chocolate alginatebeads as affected by MLE concentration (0 2 4 and 6 ww) andhardening time (2 8 and 20min) Different small letters indicatesignificant differences among samples of the same concentrationwhile different capital letters indicate significant differences amongsamples of the same hardening time at plt 005

6 Journal of Food Quality

A possible explanation would be that the loss of poly-phenols caused by prolonged hardening of the beads thatwash off from the beadsrsquo matrix was not extensive enough toaffect their radical scavenging capacity drastically

On the other hand as previously referred melanoidinsthat result from polyphenol degradation are considered thepredominant contributors of the antioxidant activity ofcocoa beans [44] e researchers of this study found thateven though TPC of roasted cocoa beans was significantlylower than that of the raw material the antioxidant activitywas the same for both samples Hence the reduction in TPCmay have not altered the antioxidant potential of the alginatebeads detrimentally

35 Sensory Evaluation Control samples and samplescontaining 6wwMLE were selected for sensory evaluationas the later presented the highest TPC and DPPH valuesIn Table 1 the scores of different sensory attributes aredisplayed In general all samples were well accepted bypanelists as values for general acceptance color tastearoma and texture ranged between 58 and 76 e ad-dition of MLE did not impart any unfavorable attributesto the samples as evidenced by similar sensory scores Nosignificant differences were detected among samplesprepared with different curing times in terms of colortaste aroma and general acceptance (plt 005) Findingsfor color are in line with those demonstrated in Figure 3showing that since curing time did not alter the colorproperties of the beads the panelists showed the sameacceptance On the other hand curing time extremes (2and 20min) negatively affected the acceptance of textureas slightly lower values were obtained for these samplesis was observed for both types of samples control andsamples with added MLE It could be therefore concludedthat chocolate beads containing 6 ww MLE cured for8min represent the sample with well-accepted sensoryattributes and most pleasant texture

4 Conclusions

Moringa oleifera leaf extract (MLE) prepared by a ldquogreenrdquoextraction technology rich in phenolic ingredients wasencapsulated in chocolate-flavored alginate beads e ap-pearance of the beads including geometric and colorproperties was affected by the amount of extract

incorporated e higher the amount of MLE added thehigher the redness yellowness and chroma of the beadswhich also became less elliptical in shape e amount ofMLE added as well as the hardening time was also critical interms of the phenolic compounds found in the final productAs a result a minimum TPC concentration of 084mg GAEg beads was established for beads prepared with 2 wwMLE allowed 20min in CaCl2 to harden However theradical scavenging activity was only concentration-relatedand a minimum 6 ww of MLE is required to enhance itsinhibitory effect e beads prepared with maximum MLEconcentration cured for 8min had the most favorable tex-ture so they can be added in food dessert products to en-hance their antioxidant potential

Data Availability

e data used to support the findings of this study are in-cluded within the article

Conflicts of Interest

e authors declare no conflicts of interest

Acknowledgments

is research has been cofinanced by the European Unionand Greek national funds through the Operational ProgramCompetitiveness Entrepreneurship and Innovation underthe call RESEARCH - CREATE - INNOVATE (project codeT1EDK-05677)

References

[1] A Rashidinejad and S M Jafari Handbook of Food Nano-technology S M Jafari Ed Academic Press Cambridge MAUSA pp 279ndash344 2020

[2] V Nedovic A Kalusevic V Manojlovic S Levic andB Bugarski ldquoAn overview of encapsulation technologies forfood applicationsrdquo Procedia Food Science vol 1 pp 1806ndash1815 2011

[3] S Castro Coelho B Nogueiro Estevinho and F RochaldquoEncapsulation in food industry with emerging electro-hydrodynamic techniques electrospinning and electro-sprayingmdasha reviewrdquo Food Chemistry vol 339 Article ID127850 2021

[4] A Lakka S Grigorakis O Kaltsa et al ldquoe effect ofultrasonication pretreatment on the production of

Table 1 Sensory evaluation scores of chocolate alginate beads (control and 6 ww MLE) prepared with different hardening times

Color Taste Aroma Texture General acceptanceControl2min 707aplusmn 088 607aplusmn 080 680aplusmn 086 653abplusmn 064 680aplusmn 0568min 713aplusmn 052 620aplusmn 077 653aplusmn 099 740cplusmn 051 700aplusmn 06520min 707aplusmn 070 627aplusmn 070 673aplusmn 046 620aplusmn 077 687aplusmn 0646 MLE2min 740aplusmn 051 627aplusmn 080 647aplusmn 074 687 bplusmn 035 707aplusmn 0468min 700aplusmn 065 580aplusmn 086 660aplusmn 099 767cplusmn 049 720aplusmn 04120min 673aplusmn 059 600aplusmn 085 633aplusmn 082 653abplusmn 052 720aplusmn 056Within the same column values followed by different letters are significantly different (plt 005)

Journal of Food Quality 7

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

A possible explanation would be that the loss of poly-phenols caused by prolonged hardening of the beads thatwash off from the beadsrsquo matrix was not extensive enough toaffect their radical scavenging capacity drastically

On the other hand as previously referred melanoidinsthat result from polyphenol degradation are considered thepredominant contributors of the antioxidant activity ofcocoa beans [44] e researchers of this study found thateven though TPC of roasted cocoa beans was significantlylower than that of the raw material the antioxidant activitywas the same for both samples Hence the reduction in TPCmay have not altered the antioxidant potential of the alginatebeads detrimentally

35 Sensory Evaluation Control samples and samplescontaining 6wwMLE were selected for sensory evaluationas the later presented the highest TPC and DPPH valuesIn Table 1 the scores of different sensory attributes aredisplayed In general all samples were well accepted bypanelists as values for general acceptance color tastearoma and texture ranged between 58 and 76 e ad-dition of MLE did not impart any unfavorable attributesto the samples as evidenced by similar sensory scores Nosignificant differences were detected among samplesprepared with different curing times in terms of colortaste aroma and general acceptance (plt 005) Findingsfor color are in line with those demonstrated in Figure 3showing that since curing time did not alter the colorproperties of the beads the panelists showed the sameacceptance On the other hand curing time extremes (2and 20min) negatively affected the acceptance of textureas slightly lower values were obtained for these samplesis was observed for both types of samples control andsamples with added MLE It could be therefore concludedthat chocolate beads containing 6 ww MLE cured for8min represent the sample with well-accepted sensoryattributes and most pleasant texture

4 Conclusions

Moringa oleifera leaf extract (MLE) prepared by a ldquogreenrdquoextraction technology rich in phenolic ingredients wasencapsulated in chocolate-flavored alginate beads e ap-pearance of the beads including geometric and colorproperties was affected by the amount of extract

incorporated e higher the amount of MLE added thehigher the redness yellowness and chroma of the beadswhich also became less elliptical in shape e amount ofMLE added as well as the hardening time was also critical interms of the phenolic compounds found in the final productAs a result a minimum TPC concentration of 084mg GAEg beads was established for beads prepared with 2 wwMLE allowed 20min in CaCl2 to harden However theradical scavenging activity was only concentration-relatedand a minimum 6 ww of MLE is required to enhance itsinhibitory effect e beads prepared with maximum MLEconcentration cured for 8min had the most favorable tex-ture so they can be added in food dessert products to en-hance their antioxidant potential

Data Availability

e data used to support the findings of this study are in-cluded within the article

Conflicts of Interest

e authors declare no conflicts of interest

Acknowledgments

is research has been cofinanced by the European Unionand Greek national funds through the Operational ProgramCompetitiveness Entrepreneurship and Innovation underthe call RESEARCH - CREATE - INNOVATE (project codeT1EDK-05677)

References

[1] A Rashidinejad and S M Jafari Handbook of Food Nano-technology S M Jafari Ed Academic Press Cambridge MAUSA pp 279ndash344 2020

[2] V Nedovic A Kalusevic V Manojlovic S Levic andB Bugarski ldquoAn overview of encapsulation technologies forfood applicationsrdquo Procedia Food Science vol 1 pp 1806ndash1815 2011

[3] S Castro Coelho B Nogueiro Estevinho and F RochaldquoEncapsulation in food industry with emerging electro-hydrodynamic techniques electrospinning and electro-sprayingmdasha reviewrdquo Food Chemistry vol 339 Article ID127850 2021

[4] A Lakka S Grigorakis O Kaltsa et al ldquoe effect ofultrasonication pretreatment on the production of

Table 1 Sensory evaluation scores of chocolate alginate beads (control and 6 ww MLE) prepared with different hardening times

Color Taste Aroma Texture General acceptanceControl2min 707aplusmn 088 607aplusmn 080 680aplusmn 086 653abplusmn 064 680aplusmn 0568min 713aplusmn 052 620aplusmn 077 653aplusmn 099 740cplusmn 051 700aplusmn 06520min 707aplusmn 070 627aplusmn 070 673aplusmn 046 620aplusmn 077 687aplusmn 0646 MLE2min 740aplusmn 051 627aplusmn 080 647aplusmn 074 687 bplusmn 035 707aplusmn 0468min 700aplusmn 065 580aplusmn 086 660aplusmn 099 767cplusmn 049 720aplusmn 04120min 673aplusmn 059 600aplusmn 085 633aplusmn 082 653abplusmn 052 720aplusmn 056Within the same column values followed by different letters are significantly different (plt 005)

Journal of Food Quality 7

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

polyphenol-enriched extracts from Moringa oleiferaL (Drumstick tree) using a novel bio-based deep eutecticsolventrdquo Applied Sciences vol 10 no 1 p 220 2020

[5] S Lalas and J Tsaknis ldquoCharacterization of Moringa oleiferaseed oil variety ldquoperiyakulam 1rdquordquo Journal of Food Compositionand Analysis vol 15 no 1 pp 65ndash77 2002

[6] A K Pandey R D Pandey P K Tripathi P P Gupta andJ Haider ldquoMoringa oleifera Lam (Sahijan)mdasha plant with aplethora of diverse therapeutic benefitsrdquo An Updated Ret-rospection Medicinal and Aromatic Plants vol 1 pp 1ndash82011

[7] S Gupta R Jain S Kachhwaha and S L Kothari ldquoNutri-tional and medicinal applications of Moringa oleifera Lam-review of current status and future possibilitiesrdquo Journal ofHerbal Medicine vol 11 pp 1ndash11 2018

[8] M Lin J Zhang and X Chen ldquoBioactive flavonoids inMoringa oleifera and their health-promoting propertiesrdquoJournal of Functional Foods vol 47 pp 469ndash479 2018

[9] M M Soliman A Aldhahrani A Alkhedaide M A NassanF Althobaiti andW AMohamed ldquoe ameliorative impactsof Moringa oleifera leaf extract against oxidative stress andmethotrexate-induced hepato-renal dysfunctionrdquo Biomedi-cine amp Pharmacotherapy vol 128 Article ID 110259 2020

[10] F Wang S Long J Zhang et al ldquoAntioxidant activities andanti-proliferative effects of Moringa oleifera L extracts withhead and neck cancerrdquo Food Bioscience vol 37 Article ID100691 2020

[11] N Hani M H Azarian A E Torkamani and W A KamilMahmood ldquoCharacterisation of gelatin nanoparticles en-capsulated with Moringa oleiferabio active extractrdquo Interna-tional Journal of Food Science amp Technology vol 51 no 11pp 2327ndash2337 2016

[12] G Batra O Gortzi S Lalas A Galidi A Alibade andG Nanos ldquoEnhanced antioxidant activity of Capsicumannuum L and Moringa oleifera L extracts after encapsu-lation in microemulsionsrdquo ChemEngineering vol 1 no 2p 15 2017

[13] A-W Lim P-Y Ng N Chieng and S-F Ng ldquoMoringa oleiferaleaf extract-loaded phytophospholipid complex for potentialapplication as wound dressingrdquo Journal of Drug Delivery Scienceand Technology vol 54 Article ID 101329 2019

[14] P Robert T Gorena N Romero E Sepulveda J Chavez andC Saenz ldquoEncapsulation of polyphenols and anthocyaninsfrom pomegranate (Punica granatum) by spray dryingrdquo In-ternational Journal of Food Science amp Technology vol 45no 7 pp 1386ndash1394 2010

[15] S Pedroso-Santana and N Fleitas-Salazar ldquoIonotropic gela-tion method in the synthesis of nanoparticlesmicroparticlesfor biomedical purposesrdquo Polymer International vol 69no 5 pp 443ndash447 2020

[16] I Donati K I Draget M Borgogna and S Paoletti ldquoTailor-made alginate bearing galactose moieties on mannuronicresidues selective modification achieved by a chemo-enzymatic strategyrdquo Biomacromolecules vol 6 no 1pp 88ndash98 2005

[17] A Dodero L Pianella S Vicini M Alloisio M Ottonelli andM Castellano ldquoAlginate-based hydrogels prepared via ionicgelation an experimental design approach to predict thecrosslinking degreerdquo European Polymer Journal vol 118pp 586ndash594 2019

[18] G A Islan and G R Castro ldquoTailoring of alginate-gelatinmicrospheres properties for oral ciprofloxacin-controlledrelease against Pseudomonas aeruginosardquo Drug Deliveryvol 21 no 8 pp 615ndash626 2014

[19] F Flamminii C D Di Mattia M Nardella et al ldquoStructuringalginate beads with different biopolymers for the developmentof functional ingredients loaded with olive leaves phenolicextractrdquo Food Hydrocolloids vol 108 Article ID 105849 2020

[20] W Zam G Bashour W Abdelwahed and W Khayata ldquoAl-ginate-pomegranate peelsrsquo polyphenols beads effects of for-mulation parameters on loading efficiencyrdquo Brazilian Journalof Pharmaceutical Sciences vol 50 no 4 pp 741ndash748 2014

[21] B Lupo A Maestro J M Gutierrez and C GonzalezldquoCharacterization of alginate beads with encapsulated cocoaextract to prepare functional food comparison of two gelationmechanismsrdquo Food Hydrocolloids vol 49 pp 25ndash34 2015

[22] T R Aguirre-Calvo S Molino M Perullini J A Rufian-Henares and P R Santagapita ldquoEffects of in vitro digestion-fermentation over global antioxidant response and shortchain fatty acid production of beet waste extracts in Ca (ii)-alginate beadsrdquo Food amp Function vol 11 no 12pp 10645ndash10654 2020

[23] A Moschona and M Liakopoulou-Kyriakides ldquoEncapsula-tion of biological active phenolic compounds extracted fromwine wastes in alginate-chitosan microbeadsrdquo Journal ofMicroencapsulation vol 35 no 3 pp 229ndash240 2018

[24] P Rijo P L Fale M L Serralheiro M F Simotildees A Gomesand C Reis ldquoOptimization of medicinal plant extractionmethods and their encapsulation through extrusion tech-nologyrdquo Measurement vol 58 pp 249ndash255 2014

[25] A Belscak-Cvitanovic R Stojanovic V Manojlovic et alldquoEncapsulation of polyphenolic antioxidants from medicinalplant extracts in alginatendashchitosan system enhanced withascorbic acid by electrostatic extrusionrdquo Food Research In-ternational vol 44 no 4 pp 1094ndash1101 2011

[26] M Franco J Beltran-Heredia and J E S Paterniani ldquoUse ofalginate-Moringa oleifera beads on Cu (II) and Cd (II) ad-sorption from aquatic systemsrdquo International Journal ofChemical Engineering and Applications vol 4 no 6pp 373ndash376 2013

[27] R Kannan S Lakshmi N Aparna S Prabhakar andW R ilagaraj ldquoEco-friendly treatment of textile dye fromaqueous solution using encapsulated biosorbent matrix beadskinetics and breakthrough analysisrdquo International Journal ofIndustrial Chemistry vol 7 no 3 pp 265ndash275 2016

[28] S E-H Asmaa A F Ehab and G H Ahmed ldquoA study of thecomparative antimicrobial activity of Moringa oleifera ex-tracts encapsulated within ALg nanoparticlesrdquoNanoscience ampNanotechnology-Asia vol 10 pp 1ndash9 2020

[29] T J Gutierrez ldquoState-of-the-art chocolate manufacture areviewrdquo Comprehensive Reviews in Food Science and FoodSafety vol 16 no 6 pp 1313ndash1344 2017

[30] A Patras ldquoStability and colour evaluation of red cabbage wastehydroethanolic extract in presence of different food additives oringredientsrdquo Food Chemistry vol 275 pp 539ndash548 2019

[31] F-H Tsai Y Kitamura and M Kokawa ldquoEffect of gumArabic-modified alginate on physicochemical propertiesrelease kinetics and storage stability of liquid-core hydrogelbeadsrdquo Carbohydrate Polymers vol 174 pp 1069ndash1077 2017

[32] A Lakka S Grigorakis I Karageorgou et al ldquoSaffron pro-cessing wastes as a bioresource of high-value added com-pounds development of a green extraction process forpolyphenol recovery using a natural deep eutectic solventrdquoAntioxidants vol 8 no 12 p 586 2019

[33] O Kaltsa S Yanniotis M Polissiou and I Mandala ldquoSta-bility physical properties and acceptance of salad dressingscontaining saffron (Crocus sativus) or pomegranate juicepowder as affected by high shear (HS) and ultrasonication

8 Journal of Food Quality

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9

(US) processrdquo LWT(Lebensmittel-Wissenschaft amp Tech-nologie) vol 97 pp 404ndash413 2018

[34] S-L Huang and Y-S Lin ldquoe size stability of alginate beadsby different ionic crosslinkersrdquo Advances in Materials Scienceand Engineering vol 2017 Article ID 9304592 7 pages 2017

[35] P Smrdel M Bogataj and A Mrhar ldquoe influence of se-lected parameters on the size and shape of alginate beadsprepared by ionotropic gelationrdquo Scientia Pharmaceuticavol 76 no 1 pp 77ndash90 2008

[36] S R Kannat S Tari and S P Chawla ldquoEncapsulation ofextract prepared from irradiated onion scales in alginatebeads a potential functional food ingredientrdquo Food Measurevol 12 pp 848ndash858 2018

[37] A Belscak -Cvitanoviv D Komes S Karlovic et al ldquoImprovingthe controlled delivery formulations of caffeine in alginatehydrogel beads combined with pectin carrageenan chitosanand psylliumrdquo Food Chemistry vol 167 pp 378ndash386 2015

[38] C D Di Mattia D Sacchetti D Mastrcola D K Sarker andP Pittia ldquoSurface properties of phenolic compounds and theirinfluence on the dispersion degree and oxidative stability of oliveoil OW emulsionsrdquo Food Hydrocolloids vol 24 no 6ndash7pp 652ndash658 2010

[39] B-B Lee P Ravindra and E-S Chan ldquoSize and shape ofcalcium alginate beads produced by extrusion drippingrdquoChemical Engineering amp Technology vol 36 no 10pp 1627ndash1642 2013

[40] W D Williams ldquoOrigin and impact of color on consumerpreference for food1rdquo Poultry Science vol 71 no 4pp 744ndash746 1992

[41] L L Garber E M Hyatt and R G Starr ldquoe effects of foodcolor on perceived flavorrdquo Journal of Marketing eory andPractice vol 8 no 4 pp 59ndash72 2000

[42] J Popov-Raljic and J Lalicic ldquoDietary chocolate colors during theirstorage up to 1 yearrdquo Journal of Agricultural Sciences vol 52 2007

[43] S Aroyeun and G Adegoke ldquoPotential of Aframomumdanielli spice powder in reducing ochratoxin A in cocoapowderrdquo American Journal of Food and Nutrition vol 1pp 155ndash165 2011

[44] C Quiroz Reyes and V Fogliano ldquoDesign cocoa processing to-wards healthy cocoa products the role of phenolics and mela-noidinsrdquo Journal of Functional Foods vol 45 pp 480ndash490 2018

[45] R Stojanovic A Belscak-Cvitanovic V ManojlovicD Komes V Nedovic and B Bugarski ldquoEncapsulation ofthyme (ymus serpyllum L) aqueous extract in calciumalginate beadsrdquo Journal of the Science of Food and Agriculturevol 92 no 3 pp 685ndash696 2012

[46] V Jost K Kobsik M Schmid and K Noller ldquoInfluence ofplasticiser on the barrier mechanical and grease resistanceproperties of alginate cast filmsrdquo Carbohydrate Polymersvol 110 pp 309ndash319 2014

[47] M Avella E D Pace B Immirizi G ImpallomeniM Malinconico and G Santagata ldquoAddition of glycerolplasticizer to seaweeds derived alginates influence of mi-crostructure on chemicalndashphysical propertiesrdquo CarbohydratePolymers vol 69 no 3 pp 503ndash511 2007

[48] A Marismandani and A Husni ldquoDevelopment and characteriza-tion of biobased alginateglycerolvirgin coconut oil as biodegrad-able packagingrdquo E3S Web of Conferences vol 147 p 03016 2020

[49] R-M Ion ldquoEvaluation of natural polyphenols entrapped incalcium alginate beads prepared by the ionotropic gelationmethodrdquo Journal of Optoelectronics and Advanced Materialsvol 15 no 7-8 pp 893ndash898 2013

Journal of Food Quality 9