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Origins and Mobility of Phosphorus Forms in theSediments of Lakes Taihu and Chaohu, ChinaQing-Hui Huang a c , Zi-Jian Wang a , Dong-Hong Wang a , Chun-Xia Wang a , Mei Ma a &Xiang-Can Jin ba State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences , The Chinese Academy of Sciences, Beijing, Chinab Research Center of Lake Environment , Chinese Research Academy of EnvironmentalSciences, Beijing, Chinac Graduate School of the Chinese Academy of Sciences , Beijing, ChinaPublished online: 06 Feb 2007.

To cite this article: Qing-Hui Huang , Zi-Jian Wang , Dong-Hong Wang , Chun-Xia Wang , Mei Ma & Xiang-Can Jin (2005) Originsand Mobility of Phosphorus Forms in the Sediments of Lakes Taihu and Chaohu, China, Journal of Environmental Science andHealth, Part A: Toxic/Hazardous Substances and Environmental Engineering, 40:1, 91-102, DOI: 10.1081/ESE-200033593

To link to this article: http://dx.doi.org/10.1081/ESE-200033593

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Journal of Environmental Science and Health, A40:91–102, 2005Copyright C© Taylor & Francis Inc.ISSN: 1093-4529 (Print); 1532-4117 (Online)DOI: 10.1081/ESE-200033593

Origins and Mobilityof Phosphorus Formsin the Sediments of LakesTaihu and Chaohu, China

Qing-Hui Huang,1, 3 Zi-Jian Wang,1,∗ Dong-Hong Wang,1

Chun-Xia Wang,1 Mei Ma,1 and Xiang-Can Jin2

1 State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, The Chinese Academy of Sciences, Beijing, China2Research Center of Lake Environment, Chinese Research Academy of EnvironmentalSciences, Beijing, China3Graduate School of the Chinese Academy of Sciences, Beijing, China

Phosphorus release from the sediment is generally an important factor for lake eutroph-ication. We have investigated phosphorus forms in surface sediments from Lake Taihuand Lake Chaohu by a chemical extraction method. The results showed that the con-centrations of Fe/Al-bound phosphorus (Fe/Al-P) and organic phosphorus (Org-P) hadsignificant correlations with those of amorphous Fe/Al oxides and organic matter in thesediments. Furthermore, Ca-bound phosphorus (Ca-P) concentrations were well relatedto total organic carbon (TOC) concentrations. The results also indicated that higher pHweakened the association of phosphates with the Fe/Al hydroxides and then resultedin Fe/Al-P release. The increase of pH was companied with autogenetic progresses ofcalcium carbonate and then elevated Ca-P concentrations in the sediments. In conclu-sion, external P loadings determine spatial distribution of P fractions, especially Fe/Al-Pand Org-P, and partially contribute to additional Ca-P fractions in these highly human-disturbed lakes. The pH-induced phosphorus mobility in the sediments is very importantfor these lakes.

Key Words: Phosphate; Phosphorus speciation; Phosphorus release; Eutrophiclakes; Yangtze River.

INTRODUCTION

Lake eutrophication is becoming a serious environmental problem in China,especially in the shallow lakes at the middle and lower reaches of the Yangtze

∗Correspondence: Zi-Jian Wang, Research Center for Eco-Environmental Sciences, TheChinese Academy of Sciences, P.O. Box 2871, Beijing 100085, P.R. China; E-mail:wangzj@mail:rcees.ac.cn.

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River.[1] Phosphorus is generally regarded as one of the key factors for the eu-trophication. As an internal source, phosphorus release from the sediment[2,3]

may contribute at an important level compared with external sources such asatmosphere deposits, agricultural runoff and wastewater discharges.[4,5] How-ever, not all of phosphorus forms are likely to be released from the sedimentand thereby render lake eutrophic.[6]

Phosphorus fractionation is a key to understanding phosphorus mobilityin the lake sediments.[7] Many chemical sequential extraction procedures[8–11]

have been applied to assess the mobility and bioavailability of phosphorus inlake sediments.[12,13] The following text describes four major P forms. Labile,loosely bound or exchangeable P fraction is easily releasable and becomes avail-able for algal growth; Fe/Al-P fraction is usually associated with Al, Fe and Mnoxides and hydroxides in the sediments; Ca-P fraction is formed from the ad-sorption of P on calcium carbonate and precipitation of calcium phosphates;organic P fraction is more complex and less understood.

Lake Taihu (area, 2300 km2; average depth, 2.1 m) and Lake Chaohu (area,750 km2; average depth, 4 m) are two major eutrophic lakes in the lower reach ofthe Yangtze River in China (Fig. 1). Excessive domestic sewages and industrialwastewaters have been discharged into the semi-enclosed bays in the north ofLake Taihu from Wuxi City,[14,15] or into the northwestern part of Lake Chaohufrom Hefei City.

However, it is not yet well established if artificial inputs affect phosphorusforms and their mobility in the sediments in these lakes. The aim of this studyis to determine the origins and mobility of phosphorus forms in the sedimentsfrom Lakes Taihu and Chaohu.

MATERIALS AND METHODS

Sampling DescriptionPrecise site locations were predetermined and corrected in situ with Mag-

ellan GPS315 (Taiwan, China). Sediment samples were collected with a Plex-iglas core sampler in Oct 2002 (autumn) and Jan 2003 (winter), respectively.The top 5-cm sediment, sliced from core sample immediately after sampling,was regarded as surface sediment sample. About 500 mL of water was retainedoverlying the core sediment; then overlying water was siphoned out withoutdisrupting the sediment surface. Water samples were filtered by polypropyleneSyringe Filter Holder (Cole Parmer, U.S.A.) with 0.45 mm Millipore celluloseacetate membrane. Sediment samples were sealed in a polyethylene zipper bagand kept in an insulated Igloo box (Aldrich Co., U.S.A.) with ice bags in thefields, and then were transported to the laboratory and were stored at −25◦Cuntil processing.

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Origins and Mobility of Phosphorus Forms 93

Figure 1: Geographic locations of Lakes Taihu and Chaohu.

Measurements for Sediment and Overlying Water SamplesElectrical conductivity (EC), pH, temperature and dissolved oxygen (DO)

of the overlying waters were measured in situ with a portable sensionTM 156Multiparameter Meter (Hach Co., U.S.A.) before filtration. The grain sizes ofthe sediments were measured using a Mastersizer 2000 Laser Size Analyzer(Malvern Co., U.K.) before freeze-dried. According to the grain sizes, we classi-fied the sediments into clay (smaller than 0.002 mm), silt (0.002–0.05 mm) andsand fractions (0.05–2 mm).[16] The following determinations (Table 1) werecarried out on the freeze-dried and abrasive sediments through a 150 µm sieve(100 meshes). Organic matter content in the sediment was estimated as theloss of ignition (LOI, % of dry weight) during the combustion at 500◦C (3 h)after having dried for 2 h at 105◦C.[17] Total organic carbon (TOC) concentra-tion in the sediment was analyzed with an Appollo 9000 TOC Analyzer (TekmarDohrman Co., U.S.A.) after pretreating the sediment samples in warm HCl 50%v/v to eliminate inorganic carbon.[18] Oxalate extractable Fe and Al (Feox,Alox),which were generally related to reactive (amorphous) oxides/hydroxides, wereextracted by 40 mL of 0.2 mol/L acid ammonium oxalate (pH 3) shaking with

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Table 1: Basic physical-chemical properties of the lake sediments.

Clay Silt Sand LOI TOC Feox AloxSites (%) (%) (%) (%) (%) (mmol/kg) (mmol/kg)

Lake TaihuT1 4.3 73.0 22.7 10.9 3.2 252.6 143.4T2 7.2 85.4 7.4 6.3 1.6 124.5 39.6T3 5.0 65.7 29.2 7.6 2.3 148.3 37.2T4 4.3 67.9 27.7 4.2 0.6 100.6 24.2T5 5.5 84.9 9.6 5.3 0.8 110.0 29.7T6 1.8 62.7 35.5 4.6 1.5 67.6 20.8

Lake ChaohuC1 10.0 84.6 5.4 8.1 — 139.1 37.8C2 6.9 70.3 22.8 7.3 1.2 183.9 45.5C3 8.0 84.7 7.4 7.7 0.8 106.0 31.5C4 6.9 59.6 33.6 2.7 — 128.3 33.8

— = no data available.

1 g of sediment for 2 h in the dark.[19] The concentrations of extractable Feand Al were determined by the inductively coupled plasma atomic emissionspectrometry (ICP-AES, HP Co., U.S.A.).

Phosphorus Fractionation for the Lake SedimentsThe different P forms in the lake sediments were analyzed by using a har-

monized protocol through inter-laboratory studies in the frame of the Stan-dards Measurements and Testing Program of the European Commission.[20]

This operationally defined scheme comprises of 3 separated extractions. First,phosphorus bound to Al, Fe, and Mn oxides/hydroxides (Fe/Al-P) was obtainedusing 1 mol/L NaOH extraction followed by the hydrolysis with 3.5 mol/L HCl,and Ca associated phosphorus (Ca-P) was extracted by 1 mol/L HCl after theNaOH extraction. In another extraction, inorganic P (Inorg-P) was extractedby 1 mol/L HCl and the residual was treated at 450◦C to decompose organicmatter and release P associated with organic matter (Org-P). Total P (TP) inthe sediment was determined by the cineration at 450◦C followed by 3.5 mol/LHCl extraction. P concentrations of the supernatant in each extraction wereanalyzed as soluble reactive P (SRP) using an ascorbic method.[21] All sampleswere analyzed in triplicate and the data were expressed as mean and stan-dard deviation. The recoveries of both inorganic P (Fe/Al-P and Ca-P, etc.) andTP (Fe/Al-P, Ca-P, and Org-P, etc.) throughout the SMT procedure were quitesatisfactory (Table 2).

RESULTS

Basic Environmental CharacteristicsIn the overlying waters, DO concentrations ranged from 5 to 7.4 mg/L in

autumn and from 9.5 to 13 mg/L in winter. Accordingly, the oxic conditions could

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Table 2: Recovery of phosphorus from the extraction procedures for lakesediments.

Recovery (%) Oct 2002 Jan 2003 SRMa

Inorganic P (Fe/Al-P + Ca-P)/Inorg-P 104.1 ± 8.8 105.5 ± 5.3 97.5Total P (Org-P + Inorg-P)/TP 104.4 ± 8.3 94.8 ± 10.2 94.7

(Fe/Al-P + Ca-P + Org-P)/TP 107.1 ± 8.3 98.2 ± 11.2 92.5aA sediment reference material (GBW07301a,1520 ± 70 mg P/g) certified by China StandardBureau.

be dominant at the sampling sites in Lakes Taihu and Chaohu between autumnand winter. The electrical conductivity was higher in the north (close to WuxiCity, Fig. 1) than in the south of Lake Taihu (Fig. 2), and it was higher at siteC1 in the northwest of Lake Chaohu (284–437 µS/cm, close to Hefei City) thanat other sites. Higher EC and lower pH values (Fig. 2) were generally relatedto wastewater discharges from the surrounding cities, e.g., Wuxi and Hefei.

With respect to the sediments, the textures at the sites of T2, T5, C1, andC3 were silt, while those at the other sites were silty loam. The concentrationsof reactive Fe and Al (Fe/Alox) in the sediments were higher at north sites thanat south sites in Lake Taihu and higher at west sites than at east sites inLake Chaohu (Table 1). In addition, organic matter and TOC concentrations

Figure 2: Variations of pH and EC in overlying waters between autumn and winter.

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Figure 3: Variations of inorganic phosphorus and total phosphorus concentrations in thelake sediments between autumn and winter.

showed similar distributions. As shown in Fig. 3, the concentrations of totalphosphorus in the sediments in the north were higher than those in the southof Lake Taihu, while those in the northwest were higher than those in the eastof Lake Chaohu. However, the concentrations of TP in most sediment showeda little variation between autumn and winter.

Phosphorus Forms in the Sediments of Lake TaihuIn Lake Taihu, the concentrations of inorganic P and organic P were higher

in the north than in the other sampling areas. Fe/Al-P concentrations (Table 3)in the north were higher than those in the middle and the southeast, wherethere were less than 100 µg/g Fe/Al-P. The spatial variation of Ca-P concen-trations showed a similar trend, but was not as obvious as that of Fe/Al-P

Table 3: Variations in major P forms in the lake sediments between autumn andwinter.

Fe/Al-P (µg/g) Ca-P (µg/g) Org-P (µg/g)

Sites Oct 2002 Jan 2003 Oct 2002 Jan 2003 Oct 2002 Jan 2003

Lake TaihuT1 2314 ± 120 1905 ± 17.1 399.4 ± 19.7 451.8 ± 9.3 317.3 ± 8.2 347.8 ± 33.5T2 228.7 ± 25.9 234.6 ± 25.6 223.5 ± 9.5 258.1 ± 6.9 167.9 ± 32.2 182.1 ± 4.6T3 445.3 ± 24.8 492.8 ± 11.9 241.3 ± 26.0 242.7 ± 6.8 242.3 ± 17.7 243.2 ± 6.8T4 55.8 ± 17.1 112.8 ± 6.6 166.3 ± 6.7 126.9 ± 2.0 108.3 ± 7.9 196.2 ± 3.5T5 95.2 ± 21.1 86.5 ± 4.6 166.0 ± 15.0 160.0 ± 3.5 158.1 ± 3.7 162.5 ± 0.7T6 50.1 ± 25.0 50.3 ± 1.5 232.0 ± 22.1 210.2 ± 3.2 94.8 ± 7.4 104.4 ± 7.9

Lake ChaohuC1 523.1 ± 10.7 531.2 ± 11.9 165.4 ± 6.4 176.8 ± 1.1 203.7 ± 15.6 217.3 ± 3.3C2 285.8 ± 6.6 324.6 ± 21.6 273.3 ± 11.9 161.0 ± 4.5 197.5 ± 16.3 205.1 ± 4.4C3 263.7 ± 26.6 166.1 ± 0.4 152.7 ± 4.8 150.1 ± 8.3 192.3 ± 3.8 180.5 ± 4.2C4 89.2 ± 11.6 170.3 ± 8.3 468.9 ± 6.5 224.3 ± 5.3 80.0 ± 6.6 194.1 ± 12.8

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concentrations. Concentrations of Org-P had smaller spatial variation in con-trast to those of Inorg-P. From autumn to winter, concentrations of Fe/Al-Pand Ca-P in the sediments had small variations in Lake Taihu, except for T1and T4. However, organic P concentrations tended to increase, especially at T4(increasing about 80%).

Phosphorus Forms in the Sediments of Lake ChaohuIn Lake Chaohu, the highest Fe/Al-P concentrations (about 530 µg/g,

Table 3) existed in the sediments at C1 in the western part, where most dis-charges of domestic and industrial wastewaters from Hefei city are received.Fe/Al-P concentrations decreased gradually in the sediments from the west tothe east. They had great variations at the sites of C3 and C4 between autumnand winter (Table 3).

The spatial variation of Ca-P concentrations in autumn was larger thanthat in winter as shown in Table 3. The variation between autumn and winterwas not obvious at C1 and C3 but great at C2 and C4. Organic P concentrationstended to decline from the west to the east of Lake Chaohu. The concentrationof Org-P at C4 in winter was greatly higher than that in autumn. No obviousseasonal variation of organic P was found at other sites.

Phosphorus Forms in Relation to the Sediment PropertiesThe concentrations of Fe/Al-bound P and organic P had significant corre-

lations with the concentrations of acid oxalate extractable Fe and Al, organicmatter and TOC (Table 4). Contrastively, Ca-bound P concentrations were onlyrelated to TOC concentrations. Andrieux-Loyer and Aminot suggested Fe/Al-Pand exchangeable P were significantly related to the proportion of fine fraction

Table 4: Correlation coefficients between phosphorus fractions andphysical-chemical properties in the sediments.

Fe/Al-P Ca-P Org-P TP

Autumn and Winter (n = 20)Fe/Al-P 1Ca-P 0.61b 1Org-P 0.83b 0.31 1TP 1.00b 0.65b 0.82b 1

Autumn (n = 10)Feox 0.86b 0.53 0.82b 0.86b

Alox 0.98b 0.52 0.77b 0.99b

Fe/Alox 0.94b 0.54 0.82b 0.94b

TOC 0.85b 0.90b 0.80b 0.85b

LOI 0.80b −0.03 0.97b 0.75a

aCorrelation is significant at the 0.05 level (two-tailed).bCorrelation is significant at the 0.01 level (two-tailed).

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(<63 µm),[22] but similar characteristics were not found in these sediments fromLakes Taihu and Chaohu (Table 4).

From Table 4, TP were highly related to Fe/Al-P, greatly attributed to theadsorption of amorphous Fe and Al oxides. Fe/Al-P concentrations had signifi-cant correlations with Org-P and Ca-P concentrations, while Ca-P was poorlyrelated to Org-P. The Org-P concentrations had significant correlations with or-ganic matter and TOC concentrations in these sediments. Similar observationswere reported in a reservoir and a river delta,[23,24] respectively. An increasein organic matter content in the sediments would lead to an increase in Org-Pconcentration.

DISCUSSION

Origins of Different P Forms in the Lake SedimentsGenerally, the electrical conductivity values are related to the concentra-

tions of major ions, strongly affected by wastewater discharges, soil leachingand/or agricultural runoff. The total phosphorus concentrations in lake waterscould be estimated from the mean depth and the conductivity.[25] Both Fe/Al-Pand organic P concentrations in the sediments had significant correlations withthe electrical conductivity (r2 = 0.60 for both, n = 20) in the overlying watersin Taihu and Chaohu, so Fe/Al-P and organic P could have important anthro-pogenic inputs. First, the wastewater discharges would enhance indirectly theassociation and adsorption of phosphates on Fe/Al oxides/hydroxides. More-over, organic matter in these sediments, mainly humic compounds and labileorganic compounds (unpublished data), was greatly affected by wastewater dis-charges and agricultural runoff. So higher Fe/Al-P percentages at T1 and C1could be mainly attributed to the wastewater discharges from the neighboringcities (Fig. 4). Therefore, the spatial variability of Fe/Al-P and Org-P in the sed-iments was controlled by the anthropogenic inputs of phosphorus in the highlyhuman-disturbed lakes.

Ca-bound phosphates could be usually derived from the detritus and hadautogenetic origins,[20] which were related to the formation of calcium phos-phate compounds and/or co-precipitation of phosphorus with calcium carbon-ate. High Ca-P percentages in the sediments of T6 and C4 (Fig. 4) were wellrelated to their high proportions of sand fraction described in Table 1. Inthese highly humandisturbed lakes, however, calcium concentrations in lakesediments should not be a dominant factor affecting the distribution of Ca-Pconcentrations for their poor correlations (unpublished data). High Ca-P con-centrations were also occurred in the sediments with high anthropogenic Pinputs (T1, T2, T3, etc.) for the formation of calcium phosphates, which wereresulted from high concentrations of calcium ion and phosphate in the overlyingwater.

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Figure 4: Triangle graphics of the percentage distribution of P forms in the lake sediment;solid points present the data in autumn and hollow points present the data in winter.

Mobility of Different P Forms in the Lake SedimentsThe Fe/Al-P concentrations had negative correlations with the pH values in

the overlying waters (r2 = −0.46, n = 20). With the increase of pH in the over-lying water (e.g., pH increasing from autumn to winter at T1 and C3; Fig. 2),ligand competition between PO3−

4 and OH− in the sediments would cause theavailability of binding sites on ferric complexes to decrease,[26,27] so the concen-trations and percentages of Fe/Al-P in the sediments would also decrease asdescribed in Table 3 and Fig. 4. Similar observations were made in the MejeanLagoon and the Biwa Lake.[28,29] Since there was a significant decrease in TPconcentration at T1 and C3 shown in Fig. 3, it could be an indication that phos-phorus mobility between two seasons could be mainly resulted from the releaseof Fe/Al-P forms. Thus, P release induced by pH increasing should be highlyregarded.

Fe/Al-P and organic P were closely correlated with each other, so organicmatter could be considered as an indirect factor of P fixation through its asso-ciation with Fe/Al hydroxides[24] as organo-clay complexes. Significant increaseof Org-P concentrations at T4 and C4 might be attributed to P fixation throughmicrobiological processes[30] in concomitant with the adsorption of Fe/Alhydroxides.

Generally, calcium phosphates would be co-precipitated with calcium car-bonate resulting from the increase in pH,[31] which could render Ca-P fractionenriched in the sediments (e.g., T1, T2, and C3 sediments) from autumn towinter (Table 3). These processes might be enhanced by additional dissolvedphosphate derived from Fe/Al-P release or anthropogenic P inputs.

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CONCLUSION

Phosphorus fractionation is a good way to understand phosphorus origins andtransformation in the sediments in the shallow lakes. The spatial variationof Fe/Al-P and organic P concentrations is greatly attributed to the variationof reactive Fe/Al and organic matter contents in Lakes Taihu and Chaohu.Therefore most Fe/Al-P and Org-P fractions are originated indirectly from thesorption of phosphates on the nascent amorphous Fe/Al oxides and organicmatter if there are many anthropogenic P inputs in these disturbed lakes. Inaddition, the artificial P inputs partially contribute to the Ca-P fractions andfurther result in the spatial variation of Ca-P concentrations in the sediments.The increase of pH will cause the mobility of phosphorus in the sediments, soour further work may consider the risk of P release with the variation of pH.

ACKNOWLEDGMENTS

This work is funded by a key project of the Chinese Academy of Sciences(Grant No. KZCX1-SW-12-II-32) and the National Key Project for Basic Re-search (Grant No. 2002CB412304).

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Received May 17, 2004

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