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Biosorption of Arsenic from Contaminated Wateronto Solid Psidium guajava Leaf Surface: Equilibrium,Kinetics, Thermodynamics, and Desorption StudySuantak Kamsonlian a , S. Suresh b , C. B. Majumder a & Shri Chand aa Department of Chemical Engineering, Indian Institute of Technology, Roorkee, Indiab Department of Chemical Engineering, Maulana Azad National Institute of TechnologyBhopal, Bhopal, M.P., India

Available online: 31 May 2012

To cite this article: Suantak Kamsonlian, S. Suresh, C. B. Majumder & Shri Chand (2012): Biosorption of Arsenic fromContaminated Water onto Solid Psidium guajava Leaf Surface: Equilibrium, Kinetics, Thermodynamics, and Desorption Study,Bioremediation Journal, 16:2, 97-112

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Bioremediation Journal, 16(2):97–112, 2012Copyright ©c 2012 Taylor and Francis Group, LLCISSN: 1088-9868DOI: 10.1080/10889868.2012.665962

Biosorption of Arsenic from ContaminatedWater onto Solid Psidium guajava Leaf

Surface: Equilibrium, Kinetics,Thermodynamics, and Desorption Study

Suantak Kamsonlian,1

S. Suresh,2 C. B. Majumder,1

and Shri Chand1

1Department of ChemicalEngineering, Indian Institute ofTechnology, Roorkee, India2Department of ChemicalEngineering, Maulana AzadNational Institute of TechnologyBhopal, Bhopal, M.P., India

ABSTRACT A batch study on the removal of As(III) and As(V) ions fromcontaminated water by biosorption using powdered Psidium guajava (Guava)leaf as biosorbent was carried out in the present work. FT-IR (Fourier transforminfrared) and SEM (scanning electron microscopy) were used to characterizethe surface of the biosorbent. The effect of sorption parameters such as pH,temperature (T c), adsorbent dose (Dc), and contact time (tc) were studied. Atoptimum treatment conditions, the maximum uptake of 1.06 mg of As(III) pergram and 2.39 mg of As(V) per gram onto the surface of biosorbent were ob-tained. Langmuir and Freundlich isotherm models were examined for sorptionequilibrium at various temperatures. The sorption isotherm was favorable withthe Freundlich model with the experimental data. Furthermore, higher uptakekinetics was tested for the pseudo-first-order and pseudo-second-order mod-els. The pseudo-second-order model appeared to be the more suitable modelto describe arsenic biosorption. �G0 values were negative at all temperatures,confirming the feasible and spontaneous nature of the biosorption process. Sol-vent desorption studies help in understanding the mechanism of the adsorptionprocess and also to check the stability of the loaded/spent adsorbents. HCl wasfound to show maximum effectiveness in the desorption of both As(III) andAs(V) with the comparison of other solvents.

KEYWORDS arsenic removal, biosorption, desorption, Psidium guajava leaf , sorptionisotherms, uptake kinetics

INTRODUCTIONIn recent decades, the widespread contamination of arsenic has been ob-

served due to natural processes and anthropogenic activities (Liangjie et al 2009;Mondal, Majumder, and Mohanty 2006; Ranjan, Talat, and Hasan 2009). Wa-ter contamination by arsenic is a global problem with high impact mainly in thepoorest regions of the Planet (Kamsonlian et al. 2011a). Several epidemiological

Address correspondence to SuantakKamsonlian, Department of ChemicalEngineering, Indian Institute ofTechnology, Roorkee-247667, India.E-mail: shoncool@gmail.com

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studies confirm the serious health hazards and chroniccarcinogenetic diseases (cancer of the bladder, lungs,skin, kidney, nasal passages, liver) and vascular diseases(Chia, Ming, and Chung 2009) such as blackfoot dis-ease and hypertension, irritations of the skin and mu-cous membranes, as well as dermatitis, keratosis, andmelanosis (Lee 2003; Choong et al. 2007) due to ar-senic pollution of water. High health risks due to ar-senic even at low concentrations leads to the limitationsof the maximum permissible limit of arsenic in Indiaand Bangladesh by 0.05 mg L−1, German 0.01 mg L−1,European Union 0.01 mg L−1, Australia 0.007 mg L−1,France 0.015 mg L−1, and Vietnam and Mexico 0.05mg L−1 (Barakat et al. 2008), whereas according to USEnvironmental Protection Agency (EPA) and WorldHealth Organization (WHO) guidelines it is 0.01 mgL−1 (Huijie et al. 2009; Arza, John, and Menachem2001). Arsenic (<0.05 mg L−1) concentrations will notexceed the permissible limit prescribed by the Bureau ofIndian Standards for drinking water (BIS 2010), whichoriginally published the BIS standard in 1983. Arsenicconcentrations in excess of 0.05 mg L−1 have beenaffected (West Bengal and Bihar states) and the pointvalues for other states (Uttar Pradesh, Assam, andChhattisgarh) based on findings of the Central GroundWater Board and Indian state agencies. The arsenic con-centration in the groundwater of West Bengal, India,lies within 0.05 to 0.2 mg L−1 (Chakraborty et al. 2002)and the relative amount of As(V) and As(III) in ground-water depends on the redox condition in the aquifer(Mohan and Pittman 2007; Mondal, Majumder, andMohanty 2009). Recently, the relative amount of As(III)and As(V) in the groundwater of some places of WestBengal has also been reported as 1:1 (Sarkar et al. 2005).As(III) is the thermodynamically stable form, which atpH values of most natural waters are presented as a non-ionic form of arsenious acid. Thus, As(III) may interactin a smaller extent with most solid surfaces, therefore,it is more difficult to be removed by the conventionaltreatment methods, such as adsorption, precipitation,etc. (Katsoyiannis, Zikoudi, and Hug 2008).

The fact that arsenic is poisonous and carcinogeneticeven at low concentration has motivated researchers todevelop various treatment technologies that have beenapplied in the removal of arsenic from waters, such ascoagulation/filtration, adsorption, ion exchange (Bartet al. 2003), reverse osmosis, nanofiltration (Balasub-ramanian, Toshinori, and Srinivasakannan 2009), elec-trocoagulation (Jewel et al. 2007), membrane filtration

(Kuan, Zaini, and Pierre 2004), chemical precipitation(Thomas et al. 1992), and biosorption for removingaqueous arsenic. Limitations in the conventional tech-nologies force to develop a new alternate for the re-moval of arsenic from aqueous solutions (Erdogan,Hatice, and Alan 2005), particularly As(III) form. Gen-erally, zero-valent iron (As(III)) in oxygen-containingwater produces reactive intermediates that can oxidizevarious organic and inorganic compounds (Katsoyian-nis, Ruettimann, and Hug 2008). Therefore, a preoxida-tion step is usually required to transform the trivalentform to pentavalent (Katsoyiannis et al. 2004). The ox-idation procedure is mainly performed by the additionof chemical reagents, such as potassium permanganate,chlorine, ozone, hydrogen peroxide, or manganese ox-ides. Iron also exerts a strong influence on arsenicconcentrations in groundwater sources, whereas ironoxides are efficient adsorbents in the arsenic removalprocesses (Katsoyiannis et al. 2004). Various treatmenttechnologies exist for removal of arsenic from wastew-ater, including precipitation, ion exchange, evapora-tion, oxidation, electroplating, and membrane filtration(Ajmal et al. 1998; Suresh, Srivastava, and Mishra2011b; Chowdhury and Saha 2011). The removal of ar-senic, such as coagulation and filtration, adsorption onactivated alumina or granular ferric hydroxide, removalduring Fe-Mn oxidation, membrane filtration, biologi-cal oxidation of Fe(II) and Mn(II), and the use of zerovalent iron (Katsoyiannis et al. 2006; Katsoyiannis, Zik-oudi, and Hug 2008). Katsoyiannis, Ruettimann, andHug (2008) reported As(III) oxidized but not removedduring the biological filtration stage. Arsenic is removedbelow 10 µg L−1 during the subsequent coagulationand filtration treatment stage. However, application ofsuch technologies is restricted because of technical oreconomical constraints (Wang and Qin 2005). Biosorp-tion as an alternative and effective technology has beenwidely studied over recent years, because of its widerange of target pollutants, high sorption capacity, ex-cellent performance, ecofriendly nature, and low op-erating cost (Kamsonlian et al. 2011b). Recent studieson biosorption have shown that common agriculturalwastes can be used as potential biosorbents for the re-moval of heavy metals (Kamsonlian et al. 2011a). Someof the authors reported their methods very effectivewhen arsenic concentrations are low, for those authorshave presumed these statements and more arsenic con-centrations were taken for evaluation purposes in thepresent study. Plant wastes are of abundance in nature

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and inexpensive (Wan et al. 2008) source as probableadsorbents. No information is, however, available in lit-erature for the removal of arsenic ions by biosorptiononto the surface of Psidium guajava leaf from contam-inated water. The objective of the present work was toinvestigate the adsorptive removal efficiency of pow-dered Psidium guajava leaf for arsenic removal fromcontaminated water. Adsorption equilibrium and ratekinetics studies were performed. Langmuir and Fre-undlich isotherms were used for sorption equilibriumstudies. The Freundlich isotherm was better fitted tothe equilibrium sorption data. Further, uptake capac-ities of biosorbent for arsenic ions were determinedunder experimental conditions.

MATERIALS AND METHODSPreparation and Characterization of

BiosorbentThe Psidium guajava leaf biomass, collected from

the institute campus of the India Institute of Technol-ogy Roorkee, India. The biosorbent was cleaned withdouble-distilled water to remove soluble lighter impuri-ties, air dried at room temperature, and then kept insidea hot air oven at a temperature of 333 K for 4 h. Thebiosorbent was coarsely grounded and sieved (ranges1.18 mm to 425 µm). Morphology of the biosorbentwas determined by using scanning electron microscopy(SEM) (Quanta, Model 200 FEG; The Netherlands).Samples were first gold coated using a sputter coater(Edwards S150), gold sputtering provides conductivityto the samples, and then SEM and simultaneouslyelemental analysis were done using an energy dispersiveX-ray spectroscopy (EDAX). Fourier transform infraredspectroscopy (FTIR) (Thermo Nicolet; Nexus, USA)was employed to determine the presence of functionalgroups in the surface of Psidium guajava. The FTIRspectrum was obtained after 32 cumulative scans bymaking KBr pellets of 1%. Physiochemical analysis wasstudied through proximate and ultimate analyses.

Preparation of Stock Solution andReagents

All the chemicals used in the present study were ofanalytical grade. For preparation of stock solutions anddilutions, double-deionized water (Millipore 17.9 M�

cm−1) was used. Stock solution of 1000 mg L−1 con-centration of As(III) was prepared by dissolving 8.2 mg

of sodium meta-arsenite (As2O3) in 1000 mL volume ofdouble deionized water. Subsequently stock solution of1000 mg L−1 concentration of As(V) was prepared byusing 8.8 mg of sodium arsenate (Na2HAsO4·7H2O).

Potassium iodide solution was prepared by dissolv-ing 15 g of potassium iodide in 100 ml of distilledwater and stored in a brown bottle. SnCl2 solutionwas prepared by dissolving 40 g of arsenic-free SnCl2in 100 ml of hydrochloric acid. Lead acetate solutionwas prepared by dissolving 10 g of lead acetate in 100ml of double distilled water. Silver diethyldithiocarba-mate (SDDC) reagent was prepared by dissolving 1 g ofSDDC in 200 ml of pyridine.

ExperimentationBatch Sorption Studies

The batch experiments were carried out in 250-mlconical flasks by adding powdered Psidium guajava leafsuspended in 100 ml of As(III) and As(V) solution sepa-rately by gently agitating the solutions in a thermostaticorbital shaker at 180 rpm. Optimizations of biosorptionparameters (pH, dosage, temperature, and contact time)were performed. To optimize various parameters, thefollowing ranges have been considered: (i) pH: 2 to 10for both arsenic species; (ii) dosage: 1 to 5 g; (iii) initialconcentration: 50 to 250 mg L−1; (iv) contact time: 0.5to 32 h; and (v) temperature: 283 to 323 K.

Analysis of Arsenic

A spectrophotometric analysis method (TashniwalTVS 25A), silver diethyl diethocarbamate (SDDC) ap-proved by IS 3025 (1988) and ASTM D 2972 (2008)was used for the analysis of arsenic solution. The de-tection limit of arsenic for SDDC method ranges from5 to 250 µg L−1 (ASTM D 2972: 2008), which alsomeets the US EPA and WHO limit for drinking waterof 10 µg L−1 (Barakat et al. 2008). As(III) speciationwas performed by the pretreatment of the samples withacids that allowed the rapid determination of inorganicarsenic species at concentrations down to 1 mg L−1.In this method; aliquots of the arsenic sample wereof necessary quantity depending upon the concentra-tion taken in the arsenic generator flask. Hydrochloricacid was added to the arsenic solution to prevail acidicconditions. KI and SnCl2 were added for the reduc-tion of As(V) to As(III). Finally, zinc dust was addedto form arsine gas, which was passed through a scrub-ber containing glass wool impregnated with lead acetate

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TABLE 1 Physiochemical Characteristics of Psidium guajava Leaf Biomass

Proximate analysis Ultimate analysis

Description % by weight Description % by weight

Moisture content 5.8 Carbon 58.2Volatile matter 61.49 Nitrogen 37.4Ash content 9.58 Hydrogen 4.4Fixed carbon 34.13 Sulfur 0

solution and then into an absorber tube containing asolution of SDDC in pyridine. Arsine reacts with thisreagent, forming a red-colored silver solution, which ismeasured photometrically at a wavelength (λ) of 540nm (Arbrab-Zavar et al. 2000).

CalculationThe amount of arsenic sorbed per unit mass of the

biosorbent (mg g−1) was evaluated by using the follow-ing equation:

qt = (Ci − Ce)VW

(1)

where C i and Ce are the arsenic concentrations(mg L−1) of initial and at equilibrium, respectively, Vis the volume of the arsenic solutions (ml), and W isthe weight of biosorbent (g).

The percentage removal was calculated by applyingthe following equation:

Removal (%) = (Ci − Cf )Ci

× 100 (2)

where C i and C f were the initial and final concentra-tions of arsenic present after the biosorption process.

RESULTS AND DISCUSSIONPhysiochemical Analysis

A 1.0034-g biosorbent sample was taken for the prox-imate analysis. Moisture content was determined bykeeping the sample at 378 K for an hour. The volatilematter was determined by keeping the sample in a cylin-drical crucible with a lid for 7 min at a temperature of723–823 K. The ash content was determined by keep-ing the sample in a flat crucible for 1 h at a temperatureof 1183 K. Fixed carbon was determined by subtractingthe moisture, volatile matter and ash content from theoriginal weight of the sample.

Table 1 represents the results of the proximate andultimate analyses. The existence of low moisture indi-cates the presence of very low fat content in Psidiumguajava leaf biomass. The presence of very high ni-trogen content relatively described the occurrence ofprotein in the biosorbent sample. On comparison ofthe results of the proximate and ultimate analyses (Ta-ble 1) with other biosorbent-citing literatures, it becameevident that the carbon content of the biosorbent wasquite high against rice husk ash and bagasse fly ash(Srivastava, Mall, and Mishra 2007). A proximate anal-ysis of the sample claimed 34.13% of carbon contenttogether with 58.2% carbon content obtained throughultimate analysis. The fixed carbon content of rice huskash and bagasse fly ash obtained through ultimate andproximate analyses were 7.42%, 16.36%, 5.90%, and19.20%, respectively. Significantly high carbon contentof Psidium guajava leaf compared to other biosorbentsshows the possibilities of Psidium guajava leaf as a verypersuasive and potent biosorbent for the removal ofmetal ions from contaminated water.

SEM and FTIR AnalysisFigure 1a represents the surface of Psidium guajava

leaf biomass, which seemed to be highly mesoporusand heterogeneous. The existence of pores and pro-trusions were not uniformly distributed, but ran in-side the biomass cell matrix. The surface roughness ofan unloaded biosorbent indicated the availability of atremendous surface area of biosorbent meant for metalion binding (Ahmad et al. 2009). Contrary to this, afterarsenic ions adsorption, the biosorbent surface seemedto have decreased porosity. This was due to have heav-ily impregnated arsenic ions onto the surface of thebiosorbent as shown in Figure 1b.

Figure 2 shows the FTIR analysis of powderedPsidium guajava leaves. The characteristic peak occursat around 1596.06 cm−1 indicating the presence ofC–C/N–C stretching. There are three characteristic

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FIGURE 1 SEM and EDX analyses of powdered Psidium guajava leaves. (a) Fresh psidium guajava; (b) loaded with As(III) ion; and(c) loaded with As(V) ion (color figure available online).

101 Biosorption of As onto P. guajava Surface

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FIGURE 2 FTIR analysis of powdered Psidium guajava leafbiomass. (A) unloaded; (B) As(V) loaded; and (C) As(III) loaded(color figure available online).

bands at around 1463.01, 1384.09, and 843.84 cm−1.The 1384.09 cm−1 band is the strongest and is relativelybroad, whereas the other two absorptions are weakerand very narrow. This indicates the presence of nitratecompounds. The CH3 asymmetric stretching vibrationoccurred at 2695.89 cm−1, whereas the CH2 absorptionoccurred at 2827.04 cm−1 (Arslanoglu, Soner Altundo-gan, and Tumen 2008; Kamsonlian et al. 2011c). Thebroad peak at 3461.11 cm−1 indicates the existence ofhydroxyl groups of macromolecular association (cellu-lose, pectin, etc.).

Effect of pH on Biosorption ofArsenic Species

The pH dependence of metal sorption was influ-enced by two factors: (i) the distribution of metal ionsin the solution phase, and (ii) the overall charge of thesorbent (Srivastava et al. 2006). The amount of sorp-tion of arsenic ions onto the biosorbent from aqueoussolution is strongly influenced by the pH value. Thedistribution of arsenic species (As(III), As(V)) in naturalwaters is mainly dependent on the redox potential andpH conditions (Cullen and Reimer 1989; Katsoyianniset al. 2007). The effect of pH on the liquid phase isof significant importance, it controls the sorption pro-cess by affecting the nature of the surface charge ofthe adsorbent at water interface and the speciation ofthe sorbate in the water (Selvakumar et al. 2010). In therange of pH 2–10, the sorption capacity of As(III) ionwas always greater than that of the As(V) ion (Figure3). A steady increase in the sorption of the As(III) ionwas seen from pH 2.0 to 6.0. The maximum specific

FIGURE 3 Effect of pH on sorption of arsenic ions (Ci, As(III) =100 mg/L; Ci, As(V) = 100 mg/L; Pc = 1.18 mm to 425 µm; Dc = 4g; tc = 8 h; rpm = 180).

uptake of 1.78 mg g−1 of the As(III) ion occurred atpH 8.0, but showed a steep reduction on higher val-ues, being As(III) ion practically uncharged up to pH8.0. As(III) may interact to a smaller extent with mostsolid surfaces and become a non-ionic form, and alsoOH radials are the main oxidant for As(III) at low pH,therefore, there is less removal, whereas a more selec-tive oxidant oxidizes As(III) at neutral pH. Thus, pH8.0 was considered as an optimum pH for the removalof As(III) ions from contaminated water. Similar re-sults were found by other researchers (Jain and Loeppert2000; Katsoyiannis and Zouboulis 2002; Mondal, Ma-jumder, and Mohanty 2009). The sorption of the As(V)ion onto the Psidium guajava leaf surface was highly pHdependent and decreased by increasing the pH from 4.0to 10.0 (Figure 3). The maximum uptake of arsenic ionsoccurred at acidic conditions. Higher uptake occurringat acidic conditions could be related to the strong elec-trostatic attraction between positively charged surfacesites for the predominant As(V) species H2AsO−

4 withpKa = 2.19, whereas a decrease in uptake of As(V) sorp-tion above pH 4 could be due to electrostatic repulsionbetween the negatively charged As(V) species, HAsO2−

4with pKb = 6.94, and the biosorbent surface (Virenderand Mary 2009). In this study we could conclude thatpH 4 as an optimum pH for As(V) ion removal.

Effect of Dosage on Biosorption ofArsenic Species

The effect of sorbent dosage on the uptake rate ofboth As(III) and As(V) ions has been represented inFigure 4, which shows that sorption efficiency increased

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FIGURE 4 Effect of sorbate dosage on adsorption of arsenic ions (Ci, As(III) = 100 mg/L; Ci, As(V) = 100 mg/L; Pc = 1.18 mm to 425 µm;pHAs(III) = 8.0; pHAs(V) = 4.0; tc = 8 h; rpm = 180).

as the dosage of sorbate was increased, since more poresand surface were available at higher dosages. The max-imum specific uptakes for sorption of arsenic speciesonto the biosorbent surface under the given experi-mental conditions were 1.93 mg g−1 for As(III) ion and1.98 mg g−1 for As(V) ion at a dosage of 4 g. An in-crease in dosage beyond 4 g results in no further uptakeof arsenic ions due to internal saturation of pores. Theoptimum adsorbent concentration for Granular Acti-vated Carbon (GAC) GAC-Cu2+ has been found to be6 g L−1, which reduces the arsenic concentration from188 to 8.5 µg L−1 (Mondal, Majumder, and Mohanty2009). Under these conditions (pH 7.2, redox 270–280mV, dissolved oxygen 2.7 mg L−1, initial iron concen-

tration of 2.8 mg L−1), removal of As(III) was around80% (Katsoyiannis, Zikoudi, and Hug 2008) and sug-gested an increase in the removal of As(III) with anincrease in dissolved oxygen.

Effect of Contact Time on Biosorptionof Arsenic Species

The contact time between the adsorbent and themetal ions is of significant importance in the treatmentof effluent by adsorption. An establishment of equilib-rium in a short period by rapid uptake of the metal ionssignifies the efficiency of the adsorbent being used inthe effluent treatment. Figure 5 represents the plot of

FIGURE 5 Effect of contact time on adsorption of arsenic ions (Ci, As(III) = 100 mg/L; Ci, As(V) = 100 mg/L; Pc = 1.18 mm to 425 µm;pHAs(III) = 8.0; pHAs(V) = 4.0; rpm = 180).

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FIGURE 6 Effect of temperature on adsorption of arsenic ions (Ci, As(III) = 100 mg/L; Ci, As(V) = 100 mg/L; Pc = 1.18 mm to 425 µm;pHAs(III) = 8.0; pHAs(V) = 4.0; rpm = 180).

the uptake capacities of As(III) and As(V) ions againstcontact time of biosorbent at initial concentration ofarsenics of 100 mg L−1, optimum pH, and temperatureconditions. A rapid uptake rate of arsenic species wasobtained at the initial stage due to the availability of alarge number of sorption sites at the onset of the pro-cess. However, the uptake capacity of sorbate becameslow and finally stabilized after 8 h. This was due to theaccumulation of arsenic species and saturation of filledactive sites (Dipu et al. 2009). The present investigationsuggests that 8 h of contact time was the optimum con-dition for the removal of arsenic ions from aqueoussolution. The maximum removal of Arsenic ions hasbeen attained in 8 h and remains constant up to 24 h(Mondal, Majumder, and Mohanty 2009) onto GAC-Cu2+ surface. Katsoyiannis et al. (2002) reported theremoval of As(V) was found to be much more efficientthan the trivalent arsenic removal with a wide rangeof initial arsenic concentrations (50–200 mg L−1) usingpolystyrene beads coated with synthetic ferrihydrite.

Effect of Temperature on Biosorptionof Arsenic Species

The influence of temperature on the sorption ca-pacity of As(III) and As(V) ions onto the surface ofpowdered Psidium guajava leaf was studied from 283 o323 K (Figure 6). In the present investigation, the ef-fect of temperature induces a positive impact on theremoval of the As(III) ion from an aqueous solution. Itwas observed that an equilibrium adsorption increasedslightly up to 303 K and optimum condition was es-

tablished at 313 K. Further, an increase in temperaturebeyond 313 K has no significant uptake capacity of theAs(III) ion from the liquid phase, which could be ex-plained by the phenomenon of desorption that takesplace as temperature increases (Mondal, Majumder, andMohanty 2008). Maximum percent removals of As(III)and As(V) was found at 303 K by Mondal, Majumder,and Mohanty (2009) onto Cu2+-impregnated granularactivated carbon.

The adsorptivity increases with the increase in tem-perature was also observed for removal of the As(V) iononto the biosorbent surface. This could be establishedby the fact that if the adsorption process is controlledby diffusion, the sorption capacity will increase withincrease in temperature, since diffusion is an endother-mic process (Srivastava et al. 2006). Though highestuptake capacity of As(V) ion has been observed at 313K, optimum temperature was established in the range of313–323 K. Thus, optimum temperature for the equi-librium adsorption of As(III) and As(V) ions was estab-lished as 313 (± 1) K, with uptake capacities of 2.10 mgg−1 for As(III) and 2.20 mg g−1 for As(V), respectively.

Sorption Isotherm ModelingThe successful representation of the dynamic sorp-

tion separation of the solute from the solution ontothe biosorbent depends upon a good description of theequilibrium separation between two phases. Differentisotherms have been used to describe the sorption equi-librium for the uptake of arsenic species on the solidsurface of the biosorbent. Langmuir and Freundlich

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FIGURE 7 Study of Langmuir isotherm for As(III) ion removal mediated by biosorption onto surface of Psidium guajava leaf (particlesize 1.18 mm, agitation rate 180 rpm, pH 8, and contact time 8 h) (color figure available online).

isotherms were tested for the present experimentalwork. The Langmuir sorption isotherm describesthat the uptake occurs on a homogeneous surface bymonolayer sorption without the interaction betweensorbed molecules (Balasubramanian, Toshinori, andSrinivasakannan 2009). It has been mathematically de-scribed as follows:

qe = K × b × Ce

1 + b × Ce(3)

The linearization of the above equation results in

Ce

qe= 1

b × KL+ Ce

KL(4)

where KL is the binding constant and b is the sorbentcapacity.

The following ranges of KL indicate the adsorptionprocess favorability, unfavorability, irreversibility, andlinear nature, i.e., (a) unfavorable biosorption: KL > 1;(b) linear biosorption: KL = 1; (c) favorable biosorp-tion: 0 < KL < 1; and (d) irreversible biosorption:KL = 0.

The Freundlich isotherm has been found to be suit-able for heterogeneous surfaces (George and Hugh1947) and for extremely low concentrations. The Fre-undlich isotherm is an empirical model relating theadsorption intensity of the sorbent towards adsorbent.The isotherm was adopted to describe the reversibleadsorption and not restricted to monolayer formation.The mathematical expression of the Freundlich model

can be expressed as

qe = Kf × C1ne (5)

The linear form of isotherm can be expressed as

log qe = log Kf + 1n

log Ce (6)

In the present investigation, the Langmuir isothermconstants (KL and b) of Equation 4 were determinedusing MATLAB software. Moreover, the Freundlichisotherm constants (K f and n) were determined by fit-ting Equation 6 to the MATLAB. Figures 7 to 10 rep-resent the isotherm curves at various temperatures andinitial concentrations varied from 50 to 250 mg L−1.Table 2 showed that Freundlich model was best suitedfor the experimental data, with high linear regressioncoefficients (R2) for both As(III) and As(V) ions at var-ious temperatures, representing that sorption occurs atmultiple layers of solid-liquid phase interaction.

Sorption KineticsKinetics of sorption refers to the velocity of adjust-

ment of the distribution equilibrium between metalbound to the biomass and metal concentration in thesurrounding fluid phase (Ranjan, Talat, and Hasan2009; Jang et al. 2010). The pseudo-first-order and

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TABLE 2 Parameters of Langmuir and Freundlich Models for the Sorption of As(III) and As(V) Ions onto the Surface of PowderedPsidium guajava Leaf

Isotherm model Temperature (K) Model parameters

Langmuir model for As(III) 283 KL = 1.089; b = .051; R2 = .978293 KL = 2.309; b = .0778; R2 = .939303 KL = 2.599; b = .132; R2 = .962313 KL = 2.818; b = .1443; R2 = .960

Langmuir model for As(V) 283 KL = 2.534; b = .0753; R2 = .948293 KL = 3.002; b = .7185; R2 = .894303 KL = 3.251; b = .096; R2 = .967313 KL = 3.254; b = .1812; R2 = .939

Freundlich model for As(III) 283 Kf = .4484; n = 3.909; R2 = .991293 Kf = .6752; n = 4.245; R2 = .990303 Kf = .9802; n = 5.19; R2 = .994313 Kf = 1.052; n = 5.045; R2 = .994

Freundlich model for As(V) 283 Kf = .698; n = 4.001; R2 = .972293 Kf = .827; n = 4.052; R2 = .989303 Kf = 1.039; n = 4.492; R2 = .990313 Kf = 1.349; n = 5.60; R2 = .990

pseudo-second-order model were used for the experi-mental data for determination of rate constants.

The Lagergren pseudo-first-order reaction model canbe expressed in linear form as

dq

dt= K1 (qe − q ) (7)

where q is the amount of metal sorbed at time t, qe

is the amount of metal sorbed at equilibrium, and k1 isthe sorption rate constant. Integrating Equation 7 forthe boundary conditions t = 0 to t = t and q = 0 toq = qt, and rearranging it for linearized data plotting,

the following equation was obtained:

log (qe − qt ) = log qe − K1

2.303t (8)

This model can be applied if log (qe − qt) versus tgives a straight line, in which case qe and k1 can be cal-culated from the intercept and slope of the plot. Resultsof the pseudo-first-order model have been representedin Figure 11 and Table 3.

FIGURE 8 Study of Freundlich isotherm model for As(III) ion removal mediated by biosorption onto surface of Psidium guajava leaf(particle size 1.18 mm, agitation rate 180 rpm, pH 4, and contact time 8 h) (color figure available online).

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FIGURE 9 Study of Langmuir isotherm for As(V) ion removal mediated by biosorption onto surface of Psidium guajava leaf (particlesize 1.18 mm, agitation rate 180 rpm, pH 8, and contact time 8 h) (color figure available online).

The pseudo-second-order reaction model can be de-scribed linearized cum integral equation as

tqt

= 1K2q 2

e+ t

qe(9)

From Equation 9 above, the reaction model constantk2 (g mg−1 h−1) and theoretical qe (mg g−1) can be ob-tained as the intercept and slope of the plot extrapolatedbetween t/qt and t. The results of the pseudo-second-order model have been represented in Figure 12 andTable 3.

FIGURE 10 Study of Freundlich isotherm for As(V) ion removal mediated by biosorption onto surface of Psidium guajava leaf (particlesize 1.18 mm, agitation rate 180 rpm, pH 4, and contact time 8 h) (color figure available online).

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FIGURE 11 Study of pseudo-first-order model at pHAs(III) = 8, pHAs(III) = 4, temperature 313 K, 180 rpm, and time range 1– 8 h.

The sorption kinetics describes the metal sorptionrate, which in turn governs the residence time of sorp-tion reaction and also the efficiency of sorption process(Pranav, Chandra, and Virendra 2006). At the initialstage, sorption performance was rapid and equilibriumafter 8 h. With the interpretation of data tabulatedin Table 3 and extrapolated in Figures 11 and 12, itbecame evident that the pseudo-second-order modelwith higher linear regression coefficient seemed to bemore proficient in explaining the reaction kinetics ofthe arsenic ions biosorption against the pseudo-first-order model with lower linear regression coefficients(R2).

The data represented in Table 4 give a significantcomparison of the uptake capacity (mg g−1) of thepresent study with various biosorbents implementedin other research findings. It was observed that thebiosorption capacity of Psidium guajava leaf was quitegood and satisfactory to use as biosorbent for removalof arsenic ions from contaminated water.

Intraparticle DiffusionA plot of qt versus t0.5 as proposed by Weber and

Morris (1963) (figure not shown) shows fitting of thedata by two linear portion for As(III) and As(V) ontoPsidium guajava leaf surface. This shows that two ormore steps influence the sorption process. The devi-ation of straight lines from the origin indicates thatthe pore diffusion is not the sole rate-controllingstep. Therefore, the adsorption proceeds via a com-plex mechanism consisting of both surface adsorptionand intraparticle transport within the pores of Psidiumguajava leaf surface. The effective diffusion coefficientof As(III) and As(V) were of the order of 2.5 × 10−10

and 2.7 × 10−10 m2/s.

Biosorption ThermodynamicsClassical thermodynamics of the adsorption pro-

cess gives the following relationship between �G0,

TABLE 3 Summary of Kinetic Model Parameters for As(III) and As(V) Ions onto the Surface of Powdered Psidium guajava Leaf at313 K

Pseudo-first-order model Pseudo-second-order model

Metal Experimental Calculated Calculatedions qe (mg g−1) qe (mg g−1) k1 (h−1) R2 qe (mg g−1) k2 (g mg−1 h−1) R2

As(III) 1.06 0.71 0.497 .950 1.04 1.84 .999As(V) 2.39 0.43 0.68 .972 1.05 1.25 .998

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FIGURE 12 Study of pseudo-second-order model at pHAs(III) = 8, pHAs(III) = 4, temperature 313 K, 180 rpm, and time range 1– 8 h.

�H0, �S0, and equilibrium adsorption constant (KD)(Suresh, Srivastava, and Mishra 2011a):

ln KD = −�G0

RT= �S0

RT− �H0

R1T

(10)

where T is the absolute temperature (K), R is the uni-versal gas constant (8.314 × 10−3 kJ mol−1 K−1), andKD ( = qe

/Ce) is the single-point or linear sorption dis-

tribution coefficient. Thus, �H0, which is the enthalpychange (kJ mol−1), can be determined from the slopeof the linear Van’t Hoff plot, i.e., lnKD versus (T −1).

Figure 13 shows the Van’t Hoff ’s plot for As(III) andAs(V), from which �H0 and �S0 values have been esti-mated (Table 5). The plot of �G0 versus T (Figure 13)

gives a straight line with the slope and intercept givingthe values of�H0 and�S0, respectively. The positive�S0 value also corresponds to an increase in the degreeof freedom of the adsorbed species (Suresh, Srivastava,and Mishra 2011a). �G0 values were negative at alltemperatures, indicating that the feasible and sponta-neous nature of the biosorption process (Suresh, Srivas-tava, and Mishra 2011a; Chowdhury and Saha 2011).Increase in value of �G0with increasing tempera-ture suggests reduction in spontaneous nature of thebiosorption process. The negative value of �H0impliesthat the biosorption is exothermic. The positive valuesof �H0 (38.48 kJ mol−1 and 14.74 kJ mol−1 for As(III)and As(V), respectively) indicate endothermic nature

TABLE 4 Comparison of Various Biosorbents Reported in Literature with Psidium guajava Leaf Maximum Uptake Capacities (qe, max)

Biosorbent/ Metal Conc. Temp. Dosage qe, max

biomass ion (mg L−1) pH (K) (g) (mg g−1) References

Coconut husk carbon As(V) 50–600 2–12 303–333 0.1 2.4 Manju et al. (1998)Activated carbon from oat hulls As(V) 0.025–0.2 5–10 — 0.015 3.08 Chuang et al. (2005)Tea fungal biomass As(III) 0.5–10 7.2 303 0.5–2.5 1.11 Murugesan et al. (2006)

As(V) 4.95Activated carbon from olive

pulp and olive stone carbonAs(III) 5–20 4.4–8.8 — 0.25 1.39 Budinova et al. (2006)

Pine wood char As(III) 0.01–0.1 3–5 278–313 10 0.0012 Mohan et al. (2007)Oak bark char As(III) 0.01–0.1 3–5 278–313 10 0.0074 Mohan et al. (2007)Immobilized sorghum biomass Arsenic 0.1–100 2–10 — 0.01 2.43 Haque et al. (2007)Moringa oleifera Lamarck seed

powderAs(V) 25 2–12 — 0.5–6 2.16 Kumari et al. (2006)

Psidium guajava leaf powder As(III) 50–250 2–10 283–323 1–5 1.06 Present studyAs(V) 2.39

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FIGURE 13 Van’t Hoff plot of adsorption equilibrium constantK for As(III) and As(V) (color figure available online).

of the adsorption process. The �H0 of As(III) is greaterthan As(V), indicating that the interaction of the Psid-ium guajava surface with As(III) is little stronger.

Desorption ExperimentThe desorption characteristics of As(III) and As(V)

from spent Psidium guajava leaf biomass were studiedusing the solvent elution shown in Figure 14. Solventdesorption studies help in understanding the mecha-nism of the adsorption process and also to check thestability of the loaded/spent adsorbents. In the solventelution study, the Psidium guajava leaf biomass utilizedfor the adsorption was separated from the solution(Suresh, Srivastava, and Mishra 2011a). The As(III)- andAs(V)-loaded Psidium guajava leaf biomass (0.2 g) wasthen agitated at 180 rpm in a series of 250-ml conicalflasks containing 50 ml of aqueous solution (0.1 N) eachof HCl, H2SO4, HNO3, distilled water, CH3COOH,

TABLE 5 Thermodynamics Parameters for the Sorption ofAs(III) and As(V) Ions onto the Surface of Powdered Psidium gua-java Leaf

Temp. KD �G0 �H0 �S0

(K) (L g−1) (kJ mol−1) (kJ mol−1) (kJ mol−1 K−1)

As(III)283 0.17 −12.41 38.48 178.41293 0.40 −14.60303 0.43 −15.31313 0.45 −15.91As(V)283 0.15 −11.71 14.74 93.49293 0.18 −12.69303 0.21 −13.58313 0.23 −14.14

FIGURE 14 Desorption efficiencies of As(III) and As(V) ion byvarious desorbing agents. T = 313 K; t = 8 h; C0 (desorbingagents) = 0.1 N; m = 40 g·L−1 (color figure available online).

C2H5OH, acetone, and NaOH of known concentra-tions at 313 K for 8 h in an orbital shaker. Under theseconditions, the metal ions were then transferred fromthe sorbents to the acid solution until a new equilib-rium was reached. HCl is found to show maximumeffectiveness in desorption of both As(III) and As(V)with the comparison of other solvents. Similar resultsshowed the biosorption of Zn(II), Cd(II), Co(II), andNi(II) onto orange peel cellulose surface (Ajmal et al.2000; Li et al. 2008). This indicates that ion exchange isinvolved in the adsorption process. Therefore, recoveryof the adsorbed metal ions and repeated usability of thebiosorbents are important in reference to the practicalapplications of treatment of industrial effluent.

ConclusionsThe present investigation indicated the potential of

Psidium guajava leaf biomass as an economically feasi-ble biosorbent for the removal of both As(III) and As(V)ions from contaminated water. The sorption of arsenicwas found to be highly pH dependent. The uptake ca-pacity of arsenic ions was increased with the increasein adsorbent dosage, initial arsenic concentration (from50 to 250 mg L−1) and with the increase in temperature(ranges 283 to 323 K). Equilibrium sorption data werefound to be well described by Freundlich isotherm.Hence sorption occurs on the heterogeneous surface

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of powdered Psidium guajava leaf and uptake capacityof arsenic ions was rapid at the initial period of batchprocess. Moreover, it was found that sorption kineticsfavor the pseudo-second-order model with high linearregression coefficients (R2

As(III) = .997 and R2As(V) =

.997) compared to the pseudo-first-order model. Thepositive values of �H0 (38.48 and 14.74 kJ mol−1 forAs(III) and As(V), respectively) indicate endothermicnature of the adsorption process. Solvent desorptionstudies help in understanding the mechanism of theadsorption process and also to check the stability of theloaded/spent adsorbents. HCl is found to show max-imum effectiveness in the desorption of both As(III)and As(V) with the comparison of other solvents.

ACKNOWLEDGMENTSThe authors would like to thank the Department of

Chemical Engineering and the Institute Instrumenta-tion Centre of Indian Institute of Technology Roorkee,India, for providing necessary facilities and to the min-istry of Human Resource Development, Governmentof India for financial support.

NOMENCLATUREb = Langmuir constant, L mg−1

Ce = Arsenic concentrations at equilibrium, mgL−1

C f = Final concentration of metal ion, mg L−1

C i = Initial concentration of metal ion, mg L−1

k1 = Pseudo-first-order rate constant, h−1

k2 = Pseudo-second-order rate constant, g mg−1

h−1

Kf = Freundlich constant, mg g−1

KL = Maximum uptake capacity, mg g−1

q = Amount of metal sorbed, mg g−1

qe = Amount of metal sorbed at equilibrium, mgg−1

qt = Adsorptive amount of adsorbate at time t,mg g−1

R2 = Regression correlation coefficientSDDC = Silver diethyldithiocarbamatet = Contact time, hT = Temperature, KV = Volume of the arsenic solutions, mlW = Weight of biosorbent, g

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