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  3. Volume 17, Number 4, 2023
  4. Investigation of the Complex Formation Process of Lead (II) with Natural Macromolecular Organic Substances (Fulvic Acids) by the Solubility and Gel Chromatographic Methods

Investigation of the Complex Formation Process of Lead (II) with Natural Macromolecular Organic Substances (Fulvic Acids) by the Solubility and Gel Chromatographic Methods

JCCT.
2023;
Volume 17, Number 4
: pp. 740 - 747
https://doi.org/10.23939/chcht17.04.740
Authors:
  1. Tamar Makharadze
  2. Giorgi Makharadze
1
Ivane Javakhishvili Tbilisi State University R.Agladze Institute of Inorganic Chemistry and Electrochemistr
2
Ivane Javakhishvili Tbilisi State University

Fulvic acids are one ofthe most important ligands, governingthe geochemical cycling of metals in the environment. The objective of the work was to investigate the complex formation process between fulvic acids and Pb(II).The complex formation processwas studied by the solubility and gel chromatographic methods at pH 5.0 and 8.0.

fulvic acids
lead fulvate
average stability constan
  1. Stevenson, F.J. Humus Chemistry: Genesis, Composition, Reactions; Wiley: New York, 1982.
  2. Sarlaki,E.; Paghaleh,A.S.; Kianmehr,M.H.; Vakilian,K.A. Chemical,Spectral and Morphologikal Characterization of Humic Acids Exsracted and Membrane Purified From Lignite. Chem. Chem. Technol. 2020, 14, 353–361. https://doi.org/10.23939/chcht14.03.353
  3. Osadchyy, V.; Nabyvanets, B.;Linnik, P.; Osadcha, N.; Nabyvanets, Y.Processes DeterminingSurface Water Chemistry; Springer International Publishing: Switzerland,2016.
  4. Makharadze, G.; Goliadze, N.; Khaiauri, A.; Makharadze, T.;Supatashvili, G. FulvicAndHumin Acids in Surface Waters of Georgia. In High-performas Polymers for Engineering-based Composites. Apple Academic Press:Waretown,NJ USA, 2016; pp 167-179.
  5. Pisarek,I.; Glowacki,M. Quality of Groundwater and Aquatic Humic Substances from Main Reservoireof Ground Water No. 333. J. Ecol. Eng. 2015,16, 46–53. https://doi.org/10.12911/22998993/60453
  6. Kovács,K.; Gáspár,A.; Sajgó, C.; Schmitt-Kopplin, P.; Tombácz, E. Comparative Study on Humic Substances Isolated in Thermal Groundwatersfrom Deep Aquifers below 700. Geochem J 2012, 46, 211-224. https://doi.org/10.2343/geochemj.1.0168
  7. Varshal,G.M.;Intskirveli,L.N.;Sirotkina,I.C.; Kolosov,I.V.;KoShcheeva,I.Y.On the Association of Fulvic Acids in Aqueous Solutions.Geokhimia1975,1581-1585.
  8. Rice,J.A.;MacCarthy,P. Statistical Evaluation of the Elemental Composition of Humic Substances.Org. Geochem. 1991, 17, 635-648.https://doi.org/10.1016/0146-6380(91)90006-6
  9. Ma,H.;Allen,H.E.;Yin,Y. Characterization of Isolated Fractions of Dissolved Organic Matter from Natural Waters and a Wastewater Effluent. Water Res.2001,35, 985-996.https://doi.org/10.1016/S0043-1354(00)00350-X
  10. Rey-Castro, C.; Mongin, S.; Huidobro, C.; David, C.; Salvador, J.;Garces, J.; Galceran,J.; Mas,F.; Puy,J. Effective Affinity Distribution for the Binding of Metal Ions to a Generic Fulvic Acid in Natural Waters.Environ. Sci. Technol.2009, 43, 7184–7191. https://doi.org/10.1021/es803006p
  11. Lenoir,T.; Manceau, A. Number of Independent Parameters in the Potentiometric Titration of Humic Substances. Langmuir2010, 26, 3998-4003.https://doi.org/10.1021/la9034084
  12. Dulaquas,G.;Waeles, M.; Gerringa, L.A.; Midag, R.; Rijkenberg, M.;Riso, R.G.The Biogeochemistry of Electroactive Humic Substances and Its Connection to Iron Chemistry in the North East Atlantic and the Western Mediterranean Sea. J. Geophys. Res: Oceans 2018,123, 5481–5499.https://doi.org/10.1029/2018JC014211
  13. Bertoli, A.C.; Garcia, J.S.; Trevisan, M.G.;Ramalho,T.C.; Matheus,P.;Freitas,M.P. Interactions fulvate-metal (Zn2+, Cu2+ and Fe2+) :Theoreticalinvestigation of thermodynamic, structuraland spectroscopic properties. Biometals2016, 29,275-285.https://doi.org/10.1007/s10534-016-9914-8
  14. Xu,H.;Xu,D.C.;Wang,Y. Natural Indices for the Chemical Hardness/Softness of Metal Cations and Ligands. ACS Omega2017, 2, 7185–7193.https://doi.org/10.1021/acsomega.7b01039
  15. Makharadze, T.; Makharadze.G.Investigation of Complex Formation Process of Copper with Macromolecular Organic Substances, Isolated from Natural Water.Organic Chemistry Plus2020,1, 1-5. https://doi.org/10.37256/ocp.112020101
  16. De Oliveira Vaz,D.; Fernandes,A.N.; Szpoganicz,B. Complexations of Divalent Metallic Ions with Fulvic Acids. Ecléticaquímica2018, 43, 54-58. https://doi.org/10.26850/1678-4618eqj.v43.1.2018.p54-58
  17. Boguta,P.; Sokolowska,Z. Zinc Binding to Fulvic acids: Assessing the Impact of pH, Metal Concentrations and Chemical Properties of Fulvic Acids on the Mechanism and Stability of Formed Soluble Complexes. Molekules2020, 25, 1297-1321.https://doi.org/10.3390/molecules25061297
  18. Wang, J.;Lü, C.; He, J; Zhao,B. Binding Characteristics of Pb2+ to Natural FulvicAcids Extracted from the Sediments in akeWuliangsuhai, inner Mongolia plateau, P.R. China. Environ Earth Sci. 2016, 75, 768-779.https://doi.org/10.1007/s12665-016-5608-3
  19. Schnitzer, M.; Skinner, S.I.M.Stability Constants of Pb, Ni, Mn, Co, Ca and Mg Fulvic AcidComplexes. Soil Sci.1967, 103, 247-252.https://doi.org/10.1097/00010694-196704000-00004
  20. Makharadze,T; Makharadze,G. Measurement of Complex Formation process of Nickel (II) with Freshwater FulvicAcidsUsing the Solubility Method.Fine Chemical Engineering2021, 2, 54-61. https://doi.org/10.37256/fce.222021870
  21. Dinu,M.; Shkinev,V.M. Complexation of Metal Ions with Organic Substances of Humus Nature: Methods of Study and Structural Features of Ligands, and Distribution of Elements between Species. Geochem. Int.2020, 58, 200–211. https://doi.org/10.1134/S0016702920020032
  22. Adusei-Gyamfi, J.; Ouddane,B.; Rietveld,L.; Cornard,J.; Criquet,J. Natural Organic Matter-Cations Complexation and its Impact on Water Treatment: A Critical Review. Water Res.2019, 160, 130-147. https://doi.org/10.1016/j.watres.2019.05.064
  23. Linnik,P.; Zhezheva,V.; Linnik,R.; Ivanchenko,Ya. Influence of the Component Composition of Organic Matter on Relationship between Dissolved Forms of Metals in the Surface Waters.Hydrobiol. J.2013,49, 91-108.https://doi.org/10.1615/HydrobJ.v49.i1.90
  24. Dudal, Y.; Gerard, F. Accounting for Natural Organic Matter in Aqueous Chemicalequilibrium Models: A Review of the Theories and Applications. Earth Sci Rev2004, 66, 199–216.https://doi.org/10.1016/j.earscirev.2004.01.002
  25. Smith, K.S.; Balistrierib, L.S.; Todd, A.S. Using Biotic Ligand Models to Predict Metal Toxicity in MineralizedSystems. Appl. Geochem. 2015, 57, 55–72.https://doi.org/10.1016/j.apgeochem.2014.07.005
  26. Balali-Mood, M.; Naseri, K.; Tahergorabi, Z.; Khazdair, M.R.; Sadeghi, M. Toxic Mechanisms of Five Heavy Metals: Mercury, Lead, Chromium, Cadmium, and Arsenic. Front. Pharmacol.2021, 12, 643972-643990. https://doi.org/10.3389/fphar.2021.643972
  27. Duruibe, J.O.; Ogwuegbu, M.O.C.; Egwurugwu, J.N. Heavy Metal Pollution andHuman Biotoxic Effects. Int. J. Phys. Sci.2007, 2, 112-118. http://www.academicjournals.org/IJPS
  28. Slaveykova,V.I; Wilkinson,K.J.; Ceresa, A.; Pretsch,E.Role of Fulvic Acid on Lead Bioaccumulation by Chlorella kesslerii.Environ. Sci. Technol.2003, 37, 1114–1121. https://doi.org/10.1021/es025993
  29. Lamelas,C.;Wilkinson,K.J.;Slaveykova,V.I. Influence of the Composition of Natural Organic Matter on Pb Bioavailability to Microalgae.Environ. Sci. Technol.2005, 39, 6109–6116.https://doi.org/10.1021/es050445t
  30. Orsetti, S.;Marco-Brown, J.L.; Andrade,E.M.; Molina,F.V. Pb (II) Binding to Humic Substances: An Equilibrium and Spectroscopic Study.Environ. Sci. Technol. 2013, 47, 8325-8333.https://doi.org/10.1021/es400999q
  31. Saar,R.A.; Weber,J.H. Lead(II)-fulvic acid complexes. Conditional Stability Constants, Solubility, and Implications for Lead(II) Mobility. Environ. Sci. Technol.1980, 14, 877–880.https://doi.org/10.1021/es60167a001
  32. Sahu, S.; Banerjee, D.K. Complexation of Copper (II), Cadmum (II) and Lead (II) with Humic and Fulvic Acidsof Yamuna River Sediments. In Chemistry for the Protection of the Environment; NY, USA, 1996; pp 375–388.
  33. Turner, D.R.; Varney, M.S.; Whitfield, M.; Mantoura, R.F.C.; Riley, J.P. Electrochemical Studies of Copper and Lead Complexation by Fulvic Acid.Geochim. Cosmochim. Acta1986,50, 289–297.https://doi.org/10.1016/0016-7037(86)90177-8
  34. Chakraborty,P.; Chakraborty,Ch.L. Competition from Cu(II), Zn(II) and Cd(II) in Pb(II) Binding to Suwannee River Fulvic Acid. Water Air Soil Pollut2008, 195, 63–71.https://doi.org/10.1007/s11270-008-9727-7
  35. Pinheiro,J.P.; Mota,A.M.; Benedetti,M.F. Lead and Calcium Binding to Fulvic Acids:  Salt Effect and Competition. Environmental.Environ. Sci. Technol. 1999,33,3398-3404. https://doi.org/10.1021/es990210f
  36. Christl, I.; Metzger, A.; Heidmann, I.; Kretzschmar, R. Effect of Humic and Fulvic Acid Concentrations and Ionic Strength on Copper and Lead Binding. Environ. Sci. Technol. 2005, 39, 5319-5326. https://doi.org/10.1021/es050018f
  37. Xiong, J.; Koopal, L.K.; Tan, W.F.; Fang, L.C.; Wang, M.X.; Zhao, W.; Liu, F.; Zhang, J.; Weng, L.P. Lead Binding to Soil Fulvicand Humic Acids: NICA-DonnanModeling and XAFS Spectroscopy. Environ. Sci. Technol.2013, 47, 11634–11642. https://doi.org/10.1021/es402123v
  38. Gondar, D.; López, R.; Fiol, S.; Antelo, J.M.; Arce, F. Cadmium, Lead, and Copper Binding to Humic Acid and Fulvic AcidExtracted from an Ombrotrophic Peat Bog. Geoderma2006, 135, 196-203.https://doi.org/10.1016/j.geoderma.2005.12.003
  39. Quan,G.;Yan,J. Binding Constants of Lead by Humicand Fulvic Acids Studied by Anodic Stripping Square Wave Voltammetry. Electrochemistry2010, 46, 90-94. https://doi.org/10.1134/S1023193510010118
  40. Gurjia, Zh.;Supatashvili, G.D.; Varshal,G.M.; Makharadze, G.A.; Chitiashvili,Z.D. Monohydrolysis of Lead Ions in Dilute Solutions. Proceedings Georgian Natl.Acad.Sci. 1992, 18, 22-26.
  41. Makharadze,G.;Supatashvili,G.;Makharadze, T. New Version of Calculation of Stability Constant of Metal-fulvate Complexes on the Example of Zinc Fulvate. Int. J. Environ. Sci. Technol.2018, 15,2165-2168. https://doi.org/10.1007/s13762-017-1576-8
  42. Beck,M.T.; Nagypal,I. Chemistry of complex equilibria;Chichester, Horwood, New York,1990.