Effective remediation of cadmium and lead contaminated soils by a novel slow-release phosphate amendment

Abstract

Phosphate is widely used to immobilize cadmium (Cd) and lead (Pb) in soils through the insoluble metal phosphate precipitation. However, an increase in the phosphorus content of the environment can cause new pollution. In this study, five slow-release phosphate amendments (SRPAs) were synthesized and their characteristics including BET, SEM, FTIR, swelling ratio, and thephosphorus release were determined. The results show that SRPA was a sphere with a network structure with a specific surface area of 5 to 7.18 m²/g andcontained phosphate, hydroxyl, carboxyl and other functional groups. Among five SRPAs, S3 sample showed good performance for phosphate release. Phosphate release from SRPA was well fitted with Ritger-Peppas model with constant n between 0.45 and 0.85, indicating that the phosphate release was in accordance with non-Fickian diffusion. As compared with monocalcium phosphate (MCP), SRPA application led to a lower concentration of water-soluble phosphorus in the soil sample and higher remediation efficiencies of Cd and Pb. The remediation efficiencies of water-soluble Cd and Pb in soil with SRPA were 97.1% and 97.9%, respectively. The remediation efficiencies of bioavailable Cd and Pb were 71.85% and 76.47%, respectively. The results of Tessier extraction showed that the exchangeable and carbonatebound fractions of Cd and Pb in the soil sample after SRPA application significantly reduced, while the residual fraction increased, indicating the stability of heavy metals increased.

Keywords

heavy metal / phosphate / slow-release amendment / soil remediation

References

[1] Álvarez-AyusoE, García-SánchezA. Sepiolite as a feasible soil additive for the immobilization of cadmium and zinc [J]. Science of the Total Environment, 2003, 305(1–3): 1-12

[2] HuangG-Y, SuX-J, RizwanM S, et al.. Chemical immobilization of Pb, Cu, and Cd by phosphate materials and calcium carbonate in contaminated soils [J]. Environmental Science and Pollution Research, 2016, 23(16): 16845-16856

[3] MignardiS, CoramiA, FerriniV. Evaluation of the effectiveness of phosphate treatment for the remediation of mine waste soils contaminated with Cd, Cu, Pb, and Zn [J]. Chemosphere, 2012, 86(4): 354-360

[4] Martínez-GómezF, GuerreroJ, MatsuhiroB, et al.. In vitro release of metformin hydrochloride from sodium alginate/polyvinyl alcohol hydrogels [J]. Carbohydrate Polymers, 2017, 155: 182-191

[5] AnithaT, KumarP S, KumarK S, et al.. Biosorption of lead(II) ions onto nano-sized chitosan particle blended polyvinyl alcohol (PVA): Adsorption isotherms, kinetics and equilibrium studies [J]. Desalination and Water Treatment, 2016, 57(29): 13711-13721

[6] ZhangD, ZhangY, ShenF, et al.. Removal of cadmium and lead from heavy metals loaded PVA — SA immobilizedLentinus edodes [J]. Desalination and Water Treatment, 2014, 52(25–27): 4792-4801

[7] MikhailovaE A, NobleR R P, PostC J. Comparison of soil organic carbon recovery by walkley-black and dry combustion methods in the Russian chernozem [J]. Communications in Soil Science and Plant Analysis, 2003, 34(1314): 1853-1860

[8] WangY-Y, YaoW-B, WangQ-W, et al.. Synthesis of phosphate-embedded calcium alginate beads for Pb(II) and Cd(II) sorption and immobilization in aqueous solutions [J]. Transactions of Nonferrous Metals Society of China, 2016, 26(8): 2230-2237

[9] JinL, LiuQ, SunZ-Y, et al.. Preparation of 5-fluorouracil/β-cyclodextrin complex intercalated in layered double hydroxide and the controlled drug release properties [J]. Industrial & Engineering Chemistry Research, 2010, 49(22): 11176-11181

[10] LawrieG, KeenI, DrewB, et al.. Interactions between alginate and chitosan biopolymers characterized using FTIR and XPS [J]. Biomacromolecules, 2007, 8(8): 2533-2541

[11] HasnainM S, NayakA K, SinghM, et al.. Alginate-based bipolymeric-nanobioceramic composite matrices for sustained drug release [J]. International Journal of Biological Macromolecules, 2016, 83: 71-77

[12] HuqT, FraschiniC, KhanA, et al.. Alginate based nanocomposite for microencapsulation of probiotic: Effect of cellulose nanocrystal (CNC) and lecithin [J]. Carbohydrate Polymers, 2017, 168: 61-69

[13] StochP, StochA, CiecinskaM, et al.. Structure of phosphate and iron-phosphate glasses by DFT calculations and FTIR/Raman spectroscopy [J]. Journal of Non-Crystalline Solids, 2016, 450: 48-60

[14] HasnainM S, NayakA K, SinghM, et al.. Alginate-based bipolymeric-nanobioceramic composite matrices for sustained drug release [J]. International Journal of Biological Macromolecules, 2016, 83: 71-77

[15] XuS-M, WuR-L, HuangX-J, et al.. Effect of the anionic-group/cationic-group ratio on the swelling behavior and controlled release of agrochemicals of the amphoteric, superabsorbent polymer poly(acrylic acid-co-diallyldimethylammonium chloride) [J]. Journal of Applied Polymer Science, 2006, 102(2): 986-991

[16] HuaS-B, MaH-Z, LiX, et al.. pH-sensitive sodium alginate/poly(vinyl alcohol) hydrogel beads prepared by combined Ca²⁺ crosslinking and freeze-thawing cycles for controlled release of diclofenac sodium [J]. International Journal of Biological Macromolecules, 2010, 46(5): 517-523

[17] SilvaD, PintoL F V, BozukovaD, et al.. Chitosan/alginate based multilayers to control drug release from ophthalmic lens [J]. Colloids and Surfaces B: Biointerfaces, 2016, 147: 81-89

[18] ZhaoL, CaoX-D, ZhengW, et al.. Copyrolysis of biomass with phosphate fertilizers to improve biochar carbon retention, slow nutrient release, and stabilize heavy metals in soil [J]. ACS Sustainable Chemistry & Engineering, 2016, 4(3): 1630-1636

[19] PedacchiaA, AdroverA. Study of release kinetics and diffusion coefficients in swellable cellulosic thin films by means of a simple spectrophotometric technique [J]. Chemical Engineering Research and Design, 2014, 92(11): 2550-2556

[20] TajarobiF, LarssonA, MaticH, et al.. The influence of crystallization inhibition of HPMC and HPMCAS on model substance dissolution and release in swellable matrix tablets [J]. European Journal of Pharmaceutics and Biopharmaceutics, 2011, 78(1): 125-133

[21] MarshallJ A, MortonB J, MuhlackR, et al.. Recovery of phosphate from calcium-containing aqueous solution resulting from biochar-induced calcium phosphate precipitation [J]. Journal of Cleaner Production, 2017, 165: 27-35

[22] SilvaD, PintoL F V, BozukovaD, et al.. Chitosan/alginate based multilayers to control drug release from ophthalmic lens [J]. Colloids and Surfaces B: Biointerfaces, 2016, 147: 81-89

[23] ChourasiyaV, BohreyS, PandeyA. Formulation, optimization, characterization and in-vitro drug release kinetics of atenolol loaded PLGA nanoparticles using 3³ factorial design for oral delivery [J]. Materials Discovery, 2016, 5: 1-13

[24] AgüeroL, Zaldivar-SilvaD, PeáaL, et al.. Alginate microparticles as oral colon drug delivery device: A review [J]. Carbohydrate Polymers, 2017, 168: 32-43

[25] CizmeciogluS C, MuezzinogluA. Solubility of deposited airborne heavy metals [J]. Atmospheric Research, 2008, 89(4): 396-404

[26] PatrickW HJr, HendersonR E. Reduction and reoxidation cycles of manganese and iron in flooded soil and in water solution [J]. Soil Science Society of America Journal, 1981, 45(5): 855-859

[27] XiaoL, GuanD-S, PeartM R, et al.. The influence of bioavailable heavy metals and microbial parameters of soil on the metal accumulation in rice grain [J]. Chemosphere, 2017, 185: 868-878

[28] Escamilla-RoaE, HuertasF J, Hernández-LagunaA, et al.. A DFT study of the adsorption of glycine in the interlayer space of montmorillonite [J]. Physical Chemistry Chemical Physics, 2017, 19(23): 14961-14971

[29] BaunD L, ChristensenT H. Speciation of heavy metals in landfill leachate: A review [J]. Waste Management & Research: the Journal of the International Solid Wastes and Public Cleansing Association, ISWA, 2004, 22(1): 3-23

[30] MaharA, WangP, LiR-H, et al.. Immobilization of lead and cadmium in contaminated soil using amendments: A review [J]. Pedosphere, 2015, 25(4): 555-568

[31] ZhongC, FengZ-X, JiangW, et al.. Evaluation of geogenic cadmium bioavailability in soil-rice system with high geochemical background caused by black shales [J]. Journal of Soils and Sediments, 2021, 21(2): 1053-1063

[32] HoubenD, EvrardL, SonnetP. Mobility, bioavailability and pH-dependent leaching of cadmium, zinc and lead in a contaminated soil amended with biochar [J]. Chemosphere, 2013, 92(11): 1450-1457

[33] SunL-N, ChenS, ChaoL, et al.. Effects of flooding on changes in Eh, pH and speciation of cadmium and lead in contaminated soil [J]. Bulletin of Environmental Contamination and Toxicology, 2007, 79(5): 514-518

[34] DingC-F, DuS-Y, MaY-B, et al.. Changes in the pH of paddy soils after flooding and drainage: Modeling and validation [J]. Geoderma, 2019, 337: 511-513

[35] KuoS, McnealB L. Effects of pH and phosphate on cadmium sorption by a hydrous ferric oxide [J]. Soil Science Society of America Journal, 1984, 48(5): 1040-1044

[36] KrishnamurtiG S R, HuangP M, KozakL M. Sorption and desorption kinetics of cadmium from soils: Influence of phosphate [J]. Soil Science, 1999, 164(12): 888-898

[37] CaoX D, MaL Q, ChenM, et al.. Impacts of phosphate amendments on lead biogeochemistry at a contaminated site [J]. Environmental Science & Technology, 2002, 36(24): 5296-5304

[38] YuH-Y, LiuC-P, ZhuJ-S, et al.. Cadmium availability in rice paddy fields from a mining area: The effects of soil properties highlighting iron fractions and pH value [J]. Environmental Pollution, 2016, 209: 38-45

[39] HammondL L, ChienS H, RoyA H, et al.. Solubility and agronomic effectiveness of partially acidulated phosphate rocks as influenced by their iron and aluminium oxide content [J]. Fertilizer Research, 1989, 19(2): 93-98

[40] BartosJ M, MullinsG L, WilliamsJ C, et al.. Water-insoluble impurity effects on phosphorus availability in monoammonium phosphate fertilizers [J]. Soil Science Society of America Journal, 1992, 56(3): 972-976

[41] YlivainioK. Effects of iron(III) chelates on the solubility of heavy metals in calcareous soils [J]. Environmental Pollution, 2010, 158(10): 3194-3200