Environmental Science and Pollution Research

, Volume 23, Issue 1, pp 351–365 | Cite as

Variation of physicochemical properties of drinking water treatment residuals and Phoslock® induced by fulvic acid adsorption: Implication for lake restoration

  • Changhui Wang
  • He-Long Jiang
  • Huacheng Xu
  • Hongbin Yin
Research Article


The use of phosphorus (P) inactivating agents to reduce internal P loading from sediment for lake restoration has attracted increasing attention. Reasonably, the physicochemical properties of P inactivating agents may vary with the interference of various environmental factors, leading to the change of control effectiveness and risks. In this study, the effect of fulvic acid (FA) adsorption on the properties of two agents, drinking water treatment residuals (DWTRs) and Phoslock®, was investigated. The results showed that after adsorption, there was little change for the main structures of DWTRs and Phoslock®, but the thermostability of Phoslock®, as well as the particle size and settleability of the two agents decreased. The specific surface area and pore volume of DWTRs also decreased, while those of Phoslock® increased. Further analysis indicated that aluminum and iron in DWTRs were stable during FA adsorption, but a substantial increase of lanthanum release from Phoslock® was observed, in particular at first (P < 0.01). Moreover, the P immobilization capability of DWTRs had little change after FA adsorption, while the capability of Phoslock® after FA adsorption decreased in solutions (P < 0.001) and sediments (P < 0.1); interestingly, from the view of engineering application, the performance of Phoslock® was not substantially affected. Overall, each P inactivating agent had its own particular responses of the physicochemical properties to environment factors, and detailed investigations on the applicability of each agent were essential before practical application.


Lake Phosphorus inactivating agent Fulvic acid Internal phosphorus loading Adsorption 

Supplementary material

11356_2015_5209_MOESM1_ESM.docx (1 mb)
ESM 1(DOCX 1062 kb)


  1. Agyin-Birikorang S, Oladeji OO, O’Connor GA, Obreza TA, Capece JC (2009) Efficacy of drinking-water treatment residual in controlling off-site phosphorus losses: a field study in Florida. J Environ Qual 38:1076–1085CrossRefGoogle Scholar
  2. Babatunde AO, Zhao YQ (2007) Constructive approaches towards water treatment works sludge management: an international review of beneficial re-uses. Crit Rev Environ Sci Technol 37:129–164CrossRefGoogle Scholar
  3. Barry MJ, Meehan BJ (2000) The acute and chronic toxicity of lanthanum to Daphnia carinata. Chemosphere 41:1669–1674CrossRefGoogle Scholar
  4. Bian S, Mudunkotuwa IA, Rupasinghe T, Grassian VH (2011) Aggregation and dissolution of 4 nm ZnO nanoparticles in aqueous environments: influence of pH, ionic strength, size, and adsorption of humic acid. Langmuir 27:6059–6068CrossRefGoogle Scholar
  5. Chen M, Ye T-R, Krumholz LR, Jiang H-L (2014) Temperature and cyanobacterial bloom biomass influence phosphorous cycling in rutrophic lake sediments. PLoS ONE 9:e93130CrossRefGoogle Scholar
  6. Erhayem M, Sohn M (2014) Stability studies for titanium dioxide nanoparticles upon adsorption of Suwannee River humic and fulvic acids and natural organic matter. Sci Total Environ 468–469:249–257CrossRefGoogle Scholar
  7. French RA, Jacobson AR, Kim B, Isley SL, Penn RL, Baveye PC (2009) Influence of ionic strength, pH, and cation valence on aggregation kinetics of titanium dioxide nanoparticles. Environ Sci Technol 43:1354–1359CrossRefGoogle Scholar
  8. Gołdyn R, Podsiadłowski S, Dondajewska R, Kozak A (2014) The sustainable restoration of lakes—towards the challenges of the water framework directive. Ecohydrol Hydrobiol 14:68–74CrossRefGoogle Scholar
  9. Gomes AFS, Lopez DL, Ladeira ACQ (2012) Characterization and assessment of chemical modifications of metal-bearing sludges arising from unsuitable disposal. J Hazard Mater 199–200:418–425CrossRefGoogle Scholar
  10. Habibiandehkordi R, Quinton JN, Surridge BWJ (2015) Long-term effects of drinking-water treatment residuals on dissolved phosphorus export from vegetated buffer strips. Environ Sci Pollut Res 22:6068–6076CrossRefGoogle Scholar
  11. Huser BJ, Pilgrim KM (2014) A simple model for predicting aluminum bound phosphorus formation and internal loading reduction in lakes after aluminum addition to lake sediment. Water Res 53:378–385CrossRefGoogle Scholar
  12. Ippolito JA, Barbarick KA, Elliott HA (2011) Drinking water treatment residuals: a review of recent uses. J Environ Qual 40:1–12CrossRefGoogle Scholar
  13. James WF (2011) Variations in the aluminum: phosphorus binding ratio and alum dosage considerations for Half Moon Lake, Wisconsin. Lake Reservoir Manage 27:128–137CrossRefGoogle Scholar
  14. Kandori K, Ishikawa T (2001) TPD–MS–TG study of hematite particles produced by the forced hydrolysis reaction. Phys Chem Chem Phys 3:2949–2954CrossRefGoogle Scholar
  15. Kleeberg A, Herzog C, Hupfer M (2013) Redox sensitivity of iron in phosphorus binding does not impede lake restoration. Water Res 47:1491–1502CrossRefGoogle Scholar
  16. Kothawala DN, Stedmon CA, Müller RA, Weyhenmeyer GA, Köhler SJ, Tranvik LJ (2014) Controls of dissolved organic matter quality: evidence from a large-scale boreal lake survey. Glob Chang Biol 20:1101–1114CrossRefGoogle Scholar
  17. Lin L, Xu X, Papelis C, Cath TY, Xu P (2014) Sorption of metals and metalloids from reverse osmosis concentrate on drinking water treatment solids. Sep Purif Technol 134:37–45CrossRefGoogle Scholar
  18. Lürling M, Tolman Y (2010) Effects of lanthanum and lanthanum-modified clay on growth, survival and reproduction of Daphnia magna. Water Res 44:309–319CrossRefGoogle Scholar
  19. Lürling M, Waajen G, van Oosterhout F (2014) Humic substances interfere with phosphate removal by lanthanum modified clay in controlling eutrophication. Water Res 54:78–88CrossRefGoogle Scholar
  20. Macias F, Caraballo MA, Nieto JM (2012) Environmental assessment and management of metal-rich wastes generated in acid mine drainage passive remediation systems. J Hazard Mater 229–230:107–114CrossRefGoogle Scholar
  21. Mackay EB, Maberly SC, Pan G, Reitzel K, Bruere A, Corker N, Douglas G, Egemose S, Hamilton D, Hatton-Ellis T, Huser B, Li W, Meis S, Moss B, Lürling M, Phillips G, Yasseri S, Spears BM (2014) Geoengineering in lakes: welcome attraction or fatal distraction? Inland Waters 4:349–356CrossRefGoogle Scholar
  22. Makris KC, Harris WG, O’Connor GA, Obreza TA, Elliott HA (2005) Physicochemical properties related to long-term phosphorus retention by drinking-water treatment residuals. Environ Sci Technol 39:4280–4289CrossRefGoogle Scholar
  23. Márquez-Pacheco H, Hansen AM, Falcón-Rojas A (2013) Phosphorous control in a eutrophied reservoir. Environ Sci Pollut Res 20:8446–8456CrossRefGoogle Scholar
  24. Meis S, Spears BM, Maberly SC, Perkins RG (2013) Assessing the mode of action of phoslock (R) in the control of phosphorus release from the bed sediments in a shallow lake (Loch Flemington, UK). Water Res 47:4460–4473CrossRefGoogle Scholar
  25. Özkundakci D, Hamilton DP, Gibbs MM (2011) Hypolimnetic phosphorus and nitrogen dynamics in a small, eutrophic lake with a seasonally anoxic hypolimnion. Hydrobiologia 661:5–20CrossRefGoogle Scholar
  26. Parfitt RL, Fraser AR, Farmer VC (1977) Adsorption on hydrous oxides. III. Fulvic acid and humic acid on goethite, gibbsite and imogolite. Eur J Soil Sci 28:289–296CrossRefGoogle Scholar
  27. Poschenrieder C, Gunsé B, Corrales I, Barceló J (2008) A glance into aluminum toxicity and resistance in plants. Sci Total Environ 400:356–368CrossRefGoogle Scholar
  28. Reedyk S, Prepas EE, Chambers PA (2001) Effects of single Ca(OH)2 doses on phosphorus concentration and macrophyte biomass of two boreal eutrophic lakes over 2 years. Freshw Biol 46:1075–1087CrossRefGoogle Scholar
  29. Reitzel K, Hansen J, Jensen HS, Andersen FØ, Hansen KS (2003) Testing aluminum addition as a tool for lake restoration in shallow, eutrophic Lake Sønderby, Denmark. Hydrobiologia 506:781–787CrossRefGoogle Scholar
  30. Reitzel K, Andersen FØ, Egemose S, Jensen HS (2013a) Phosphate adsorption by lanthanum modified bentonite clay in fresh and brackish water. Water Res 47:2787–2796CrossRefGoogle Scholar
  31. Reitzel K, Lotter S, Dubke M, Egemose S, Jensen HS, Andersen FØ (2013b) Effects of Phoslock® treatment and chironomids on the exchange of nutrients between sediment and water. Hydrobiologia 703:189–202CrossRefGoogle Scholar
  32. Salman M, El-Eswed B, Khalili F (2007) Adsorption of humic acid on bentonite. Appl Clay Sci 38:51–56CrossRefGoogle Scholar
  33. Spears BM, Lürling M, Yasseri S, Castro-Castellom AT, Gibbs M, Meis S, McDonald C, Mclntosh J, Sleep D, van Oosterhout F (2013a) Lake responses following lanthanum-modified bentonite clay (Phoslock®) application: an analysis of water column lanthanum data from 16 case study lakes. Water Res 47:5930–5942CrossRefGoogle Scholar
  34. Spears BM, Meis S, Anderson A, Kellou M (2013b) Comparison of phosphorus (P) removal properties of materials proposed for the control of sediment p release in UK lakes. Sci Total Environ 442:103–110CrossRefGoogle Scholar
  35. Spears BM, Maberly SC, Pan G, Mackay E, Bruere A, Corker N, Douglas G, Egemose S, Hamilton D, Hatton-Ellis T, Huser B, Li W, Meis S, Moss B, Lürling M, Phillips G, Yasseri S, Reitzel K (2014) Geo-engineering in lakes: a crisis of confidence? Environ Sci Technol 48:9977–9979CrossRefGoogle Scholar
  36. Sunding MF, Hadidi K, Diplas S, Løvvik OM, Norby TE, Gunnæs AE (2011) XPS characterisation of in situ treated lanthanum oxide and hydroxide using tailored charge referencing and peak fitting procedures. J Electron Spectrosc 184:399–409CrossRefGoogle Scholar
  37. Tang W-W, Zeng G-M, Gong J-L, Liang J, Xu P, Zhang C, Huang B-B (2014) Impact of humic/fulvic acid on the removal of heavy metals from aqueous solutions using nanomaterials: a review. Sci Total Environ 468–469:1014–1027CrossRefGoogle Scholar
  38. Tinnacher RM, Nico PS, Davis JA, Honeyman BD (2013) Effects of fulvic acid on uranium (VI) sorption kinetics. Environ Sci Technol 47:6214–6222Google Scholar
  39. USEPA (2007) SW-846 method 3051: microwave assisted acid digestion of sediments, sludges, soils and oils. U S Environmental Protection Agency, Washington DCGoogle Scholar
  40. USEPA (2008) Fate, transport and transformation test guidelines: OPPTS 835. 1230—adsorption/desorption (batch equilibrium). U S Environmental Protection Agency, Washington DCGoogle Scholar
  41. van Oosterhout F, Lürling M (2011) Effects of the novel 'Flock & Lock' lake restoration technique on Daphnia in Lake Rauwbraken (the Netherlands). J Plankton Res 33:255–263CrossRefGoogle Scholar
  42. van Oosterhout F, Lürling M (2013) The effect of phosphorus binding clay (Phoslock®) in mitigating cyanobacterial nuisance: a laboratory study on the effects on water quality variables and plankton. Hydrobiologia 710:265–277CrossRefGoogle Scholar
  43. Wang S, Yi W, Yang S, Jin X, Wang G, Wu F (2011) Effects of light fraction organic matter removal on phosphate adsorption by lake sediments. Appl Geochem 26:286–292CrossRefGoogle Scholar
  44. Wang CH, Qi Y, Pei YS (2012a) Laboratory investigation of phosphorus immobilization in lake sediments using water treatment residuals. Chem Eng J 209:379–385CrossRefGoogle Scholar
  45. Wang CH, Wang ZY, Lin L, Tian BH, Pei YS (2012b) Effect of low molecular weight organic acids on phosphorus adsorption by ferric-alum water treatment residuals. J Hazard Mater 203–204:145–150CrossRefGoogle Scholar
  46. Wang CH, Gao SJ, Pei YS, Zhao YQ (2013a) Use of drinking water treatment residuals to control the internal phosphorus loading from lake sediments: laboratory scale investigation. Chem Eng J 225:93–99CrossRefGoogle Scholar
  47. Wang CH, Liang JC, Pei YS, Wendling LA (2013b) A method for determining the treatment dosage of drinking water treatment residuals for effective phosphorus immobilization in sediments. Ecol Eng 60:421–427CrossRefGoogle Scholar
  48. Wang CH, Yuan NN, Pei YS (2014) An anaerobic incubation study of metal lability in drinking water treatment residue with implications for practical reuse. J Hazard Mater 274:342–348CrossRefGoogle Scholar
  49. Yamashita T, Hayes P (2008) Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials. Appl Surf Sci 254:2441–2449CrossRefGoogle Scholar
  50. Yan M, Dryer D, Korshin GV, Benedetti MF (2013) In situ study of binding of copper by fulvic acid: comparison of differential absorbance data and model predictions. Water Res 47:588–596CrossRefGoogle Scholar
  51. Yang Y, Zhao YQ, Kearney P (2008) Influence of ageing on the structure and phosphate adsorption capacity of dewatered alum sludge. Chem Eng J 145:276–284CrossRefGoogle Scholar
  52. Yang M, Lin J, Zhan Y, Zhu Z, Zhang H (2015) Immobilization of phosphorus from water and sediment using zirconium-modified zeolites. Environ Sci Pollut Res 22:3606–3619CrossRefGoogle Scholar
  53. Yuan CG, Shi JB, He B, Liu JF, Liang LN, Jiang GB (2004) Speciation of heavy metals in marine sediments from the East China Sea by ICP-MS with sequential extraction. Environ Int 30:769–783CrossRefGoogle Scholar
  54. Zamparas M, Zacharias I (2014) Restoration of eutrophic freshwater bymanaging internal nutrient loads. A review. Sci Total Environ 496:551–562CrossRefGoogle Scholar
  55. Zhao YQ, Zhao XH, Babatunde AO (2009) Use of dewatered alum sludge as main substrate in treatment reed bed receiving agricultural wastewater: long-term trial. Bioresour Technol 100:644–648CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  • Changhui Wang
    • 1
  • He-Long Jiang
    • 1
  • Huacheng Xu
    • 1
  • Hongbin Yin
    • 1
  1. 1.State Key Laboratory of Lake Science and Environment, Nanjing Institute of Geography and LimnologyChinese Academy of SciencesNanjingChina

Personalised recommendations