Immobilizing remediation of arsenic and cadmium in contaminated soil using an FeMnNi-LDH composite modified by fulvic acid
HE Ya-xin, WEI Shi-qiang, JIANG Zhen-mao
Chongqing Key Laboratory of Agricultural Resources and Environment Research, College of Resources and Environment, Southwest University, Chongqing 400715, China
Abstract:In this study, a stable layered FA@FeMnNi-LDH composite was prepared by co-precipitation method using fulvic acid as the modifier of FeMnNi-LDH, which was applied for the concurrent immobilization of As (III) and Cd (II) in polluted soil. Taking the Chinese cabbage (Brassica rapa pekinensis) as test crop, the effects of the composite on the remediation efficiencies of soil As (III) and Cd (II), their transformation in soils and transport and enrichment coefficients in crop plants were studied by pot experiments under different levels pollution levels of As and Cd and initial soil pH. The results showed that the synthesized composite exhibited remarkable synchronous immobilizing effects for As and Cd in soil. The application of the composite at a dosage of 1.0% promoted the both transformations of soil As and Cd from active forms to less liable forms: from non-specific adsorbed and crystalline iron aluminum oxide bound forms to specific adsorbed and amorphous iron aluminum oxide bound and residual forms for As and exchangeable form to residual, carbonate bound, iron manganese oxide bound and organic bound forms for Cd. Meanwhile, the initial soil pH values exhibited significant impacts on the immobilizing effect of As and Cd. 1% addition of the composite increased the soil pH by 1.65 and 0.64 units for acidic and neutral soils, respectively. Accordingly, soil available As and Cd contents were deceased by 69.74% and 63.31% and 60.25% and 61.78%, respectively. The fresh weight and plant height of Chinese cabbage increased with the increase of composite material addition, while the transport and enrichment coefficient of As and Cd in each part of tested crop decreased significantly. Consequently, the concentrations of As and Cd in the above-ground part of the crop were lower than the Chinese national food safety standard limit at 1% addition rate of the composite. Correlation analyses showed that non-specific adsorbed As and exchangeable Cd were negatively correlated with soil pH value, the residual As and Cd were positively correlated with soil pH value, and the contents of As and Cd in the ground part and roots of the tested crop were negatively correlated with the residual As and Cd. The results proved that FA@FeMnNi-LDH composite material could increase soil
何雅馨, 魏世强, 蒋珍茂. 富里酸改性FeMnNi-LDH对砷镉污染土壤的钝化修复[J]. 中国环境科学, 2024, 44(4): 2184-2197.
HE Ya-xin, WEI Shi-qiang, JIANG Zhen-mao. Immobilizing remediation of arsenic and cadmium in contaminated soil using an FeMnNi-LDH composite modified by fulvic acid. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(4): 2184-2197.
[1] Maziarz P, Matusik J, Strączek T, et al. Highly effective magnet-responsive LDH-Fe oxide composite adsorbents for As(V) removal[J]. Chemical Engineering Journal, 2019,326:207-216. [2] Zhou J, Shu W, Gao Y, et al. Enhanced arsenite immobilization via ternary layered double hydroxides and application to paddy soil remediation[J]. RSC Advances, 2017,7(33):20320-20326. [3] 李英,商建英,黄益宗,等.镉砷复合污染土壤钝化材料研究进展[J]. 土壤学报, 2021,58(4):837-850. Li Y, Shang J Y, Huang Y Z, et al. Research progress on passivation materials for cadmium-arsenic co-contamination in soil[J]. Acta Pedologica Sinica, 2021,58(4):837-850. [4] Wang Q W, Lin Q H, Li Q Z, et al. As (III) removal from wastewater and direct stablilization by in-situ formation of Zn-Fe layered double hydroxides[J]. Journal of Hazardous Materials, 2021,403,doi:10.1016/j.jhazmat. 2020.123920. [5] Asiabi H, Yamini Y, Shamsayei M, et al. Highly selective and efficient removal and extraction of heavy metals by layered double hydroxides intercalated with the diphenylamine-4-sulfonate:a comparative study[J]. Chemical Engineering Journal, 2017,323:212-223. [6] Li H, Yang Z L, Dai M W, et al. Input of Cd from agriculture phosphate fertilizer application in China during 2006~2016[J]. Science of The Total Environment, 2020,716:135448. [7] Zhang X Y, Chen D M, Zhong T Y, et al. Assessment of cadmium (Cd) concentration in arable soil in China[J]. Environmental Science and Pollution Research, 2015,22(7):4932-4941. [8] 杨淑华,王台,钱前,等.2015年中国植物科学若干领域重要研究进展[J]. 植物学报, 2016,51(4):416-472. YANG S H, WANG T, QIAN Q, et al. Research Advances on Plant Science in China in 2015. Chinese Bulletin of Botany, 2016,51(4):416-472. [9] Zeng Q B, Zhang A H. Assessing potential mechanisms of arsenic-induced skin lesions and cancers:human and in vitro evidence[J] Environmental Pollution, 2020,260:113919. [10] Liu Q Q, Leslie E M, Moe B, et al. Metabolism of a phenylarsenical in human hepatic cells and identification of a new arsenic metabolite[J]. Environmental Science & Technology, 2018,52(3):1386-1392. [11] Yu H Y, Ding X D, Li F B, et al. The availabilities of arsenic and cadmium in rice paddy fields from a mining area:The role of soil extractable and plant silicon[J]. Environmental Pollution, 2016,215:258-265. [12] Zhao F J. Strategies to manage the risk of heavy metal(loid) contamination in agricultural soils[J]. Frontiers of Agricultural Science and Engineering, 2020,7(3):333-338. [13] Wang L, Li Z T, Wang Y, et al. Performance and mechanisms for remediation of Cd(II) and As(III) co-contamination by magnetic biochar-microbe biochemical composite:Competition and synergy effects[J]. Science of The Total Environment, 2020,750:141672. [14] 曹勤英,黄志宏.污染土壤重金属形态分析及其影响因素研究进展[J]. 生态科学, 2017,36(6):222-232. CAO Q Y, HUANG Z H. Review on speciation analysis of heavy metals in polluted soils and its influencing factors[J]. Ecological Science, 2017,36(6):222-232. [15] 何雅馨,柯心怡,魏世强,等.富里酸改性FeMnNi-LDH复合材料对水中砷镉的吸附性能与机制.环境科学, 2023,44(5):2646-2660. He Y X, Ke X Y, Wei S Q, et al. Adsorption Characteristics of Arsenic and Cadmium by FeMnNi-LDH Composite Modified by Fulvic Acid and Its Mechanisms. Environmental Science, 2023,44(5):2646-2660. [16] 鲍士旦.土壤农化分析(第三版)[M]. 北京:中国农业出版社, 2002. [17] GB 15618-2018土壤环境质量农用地土壤污染风险管控标准(试行)[S]. [18] Fedotov P S, Fitz W J, Wennrich R, et al. Fractionation of arsenic in soil and sludge samples:continuous-flow extraction using rotating coiled columns versus batch sequential extraction[J]. Analytica Chimica Acta, 2005,538:93-98. [19] Yang Z B, Guo W Q, Cheng Z, et al. Possibility of using combined compost-attapulgite for remediation of Cd contaminated soil[J]. Journal of Cleaner Production, 2022,368:133216. [20] Alexander P D, Alloway B J, Dourado A M. Genotypic variations in the accumulation of Cd, Cu, Pb and Zn exhibited by six commonly grown vegetables. Environmental Pollution, 2006,144:736-745. [21] Jawad A, Peng L, Liao Z W, et al. Selective removal of heavy metals by hydrotalcites as adsorbents in diverse wastewater:Different intercalated anions with different mechanisms[J]. Journal of Cleaner Production, 2019,211:1112-1126. [22] Wang P, Yin L, Wang X, et al. L-cysteine intercalated layered double hydroxide for highly efficient capture of U(VI) from aqueous solutions[J]. Journal of Environmental Management, 2018,217:468-477. [23] Kabiri S, Tran D N, Azari S, et al. Graphene-diatom silica aerogels for efficient removal of mercury ions from water[J]. ACS Applied Materials & Interfaces 2015,7(22):11815-11823. [24] Hakami O, Zhang Y, Banks C J. Thiol-functionalised mesoporous silica-coated magnetite nanoparticles for high efficiency removal and recovery of Hg from water[J]. Water Research, 2012,46(12):3913-3922. [25] Xu H, Yuan Y, Liao Y, et al.[MoS4]2- Cluster bridges in Co-Fe layered double hydroxides for mercury uptake from S-Hg mixed flue gas[J]. Environmental Science and Technology, 2017,51(17):10109-10116. [26] Shamsayei M, Yamini Y, Asiabi H. Evaluation of reusable organic-inorganic nafion/layered double hydroxide nanohybrids for highly efficient uptake of mercury ions from aqueous solution[J]. Applied Clay Science, 2018,162:534-542. [27] Dai X, Zhang S, Waterhouse G, et al. Recyclable polyvinyl alcohol sponge containing flower-like layered double hydroxide microspheres for efficient removal of As(V) anions and anionic dyes from water[J]. Journal of Hazardous Materials, 2019,367:286-292. [28] Ma L, Wang Q, Islam S M, et al. Highly selective and efficient removal of heavy metals by layered double hydroxide intercalated with the MoS42- Ion[J]. Journal of the American Chemical Society, 2016,138(8):2858-2866. [29] Yan C Y, Wen J, Wang Q, et al. Mobilization or immobilization? The effect of HDTMA-modified biochar on As mobility and bioavailability in soil[J]. Ecotoxicology and Environmental Safety, 2021,207:111565. [30] Liu Q J, Li X, Tang J P, et al. Characterization of goethite-fulvic acid composites and their impact on the immobility of Pb/Cd in soil[J]. Chemosphere, 2019,222:556-563. [31] Yang Z H, Gong H Y, He F S, et al. Iron-doped hydroxyapatite for the simultaneous remediation of lead-, cadmium- and arsenic-co-contaminated soil[J]. Environmental Pollution, 2022,312:119953. [32] 王义祥,赖永翔,叶菁,等.生物炭对不同镉污染土壤钝化效果和小白菜镉吸收的影响[J]. 土壤通报, 2019,50(3):713-718. Wang Y X, Lai Y X, Ye J, et al. Effects of biochar on passivation and uptake of cadmium by Brassica chinensis in cadmium-polluted soils[J]. Chinese Journal of Soil Science, 2019,50(3):713-718. [33] Wang M, Zhu Y, Cheng L, et al. Review on utilization of biochar for metal-contaminated soil and sediment remediation[J]. Journal of Environmental Sciences, 2018,63:156-173. [34] Li D Q, Lai C H, Li Y T, et al. Biochar improves cd-contaminated soil and lowers Cd accumulation in Chinese flowering cabbage (Brassica parachinensis L.)[J]. Soil & Tillage Research, 2021,213:105085. [35] Santos R M M, Gonçalves R G L, Constantino V R L, et al. Adsorption of Acid Yellow 42Dye on Calcined Layered Double Hydroxide:Effect of Time, Concentration, pH and Temperature[J]. Applied Clay Science, 2017,140:132-139. [36] Ding C, Zhou F, Li X, et al. Modeling the transfer of arsenic from soil to carrot (Daucus carota L.)-a greenhouse and field-based study[J]. Environmental Science and Pollution Research, 2015,22:10627-10635. [37] Honma T, Ohba H, Kaneko-Kadokura A, et al. Optimal soil Eh, pH, and water management for simultaneously minimizing arsenic and cadmium concentrations in rice grains[J]. Environmental Science & Technology, 2016,50(8):4178-4185. [38] Tang J, Zhang L, Zhang J, et al. Physicochemical features, metal availability and enzyme activity in heavy metal-polluted soil remediated by biochar and compost[J]. Science of the Total Environment, 2020,701:134751. [39] Gu J F, Zhou H, Tang H, et al. Cadmium and arsenic accumulation during the rice growth period under in situ remediation[J]. Ecotoxicology and Environmental Safety, 2019,171:451-459. [40] Hudcova B, Veselska V, Filip J, et al. Sorption mechanisms of arsenate on Mg-Fe layered double hydroxides:A combination of adsorption modeling and solid state analysis[J]. Chemosphere, 2017,168:539-548. [41] Hinkle M A G; Dye K G, Catalano, J G, et al. Impact of Mn(II)-manganese oxide reactions on Ni and Zn speciation[J]. Environmental Science & Technology, 2017,51(6):3187-3196. [42] Dong Y, Lin H, Zhao Y, et al. Remediation of vanadium-contaminated soils by the combination of natural clay mineral and humic acid[J]. Journal Of Cleaner Production, 2021,279:123874. [43] Wu W L, Liu Z H, Azeem M, et al. Hydro xyapatite tailored hierarchical porous biochar composite immobilized Cd(II) and Pb(II) and mitigated their hazardous effects in contaminated water and soil[J]. Journal of Hazardous Materials, 2022,437:129330. [44] Awad Y M, Vithanage M, Niazi N K, et al. Potential toxicity of trace elements and nanomaterials to Chinese cabbage in arsenic- and lead-contaminated soil amended with biochars[J]. Environmental Geochemistry and Health, 2019,41:1777-1791. [45] Martin M, Bonifacio E, Barberis, E, et al. Arsenic fixation and mobilization in the soils of the Ganges and Meghna floodplains. Impact of pedoenvironmental properties[J]. Geoderma, 2014,228:132-141. [46] Fairbrother A, Wenstel R, Sappington K, et al. Framework for metals risk assessment[J]. Ecotoxicology and Environmental Safety, 2007, 68:145-227. [47] Chen D, Liu X Y, Bian R J, et al. Effects of biochar on availability and plant uptake of heavy metals -A meta-analysis[J]. Journal of Environmental Management, 2018,222:76-85. [48] Chou M L, Jean J S, Yang C M, et al. Inhibition of ethylenediaminetetraacetic acid ferric sodium salt (EDTA-Fe) and calcium peroxide (CaO2) on arsenic uptake by vegetables in arsenic-rich agricultural soil[J]. Journal of Geochemical Exploration, 2016, 163:19-27. [49] GB 2762-2012食品中污染物限量标准[S]. [50] Liu K, Lv J L, He W X, et al. Major factors influencing cadmium uptake from the soil into wheat plants[J]. Ecotoxicology and Environmental Safety, 2015,113:207-213. [51] 沈浩然.稻麦轮作体系下不同钝化材料对土壤镉砷复合污染修复研究[D]. 杭州:浙江大学, 2019. [52] Zhou R, Liu X, Luo L, et al. Remediation of Cu, Pb, Zn and Cd-contaminated agricultural soil using a combined red mud and compost amendment[J]. International Biodeterioration & Biodegradation, 2017,118:73-81. [53] Lahori A H, Zhang Z Q, Guo Z Y, et al. Beneficial effects of tobacco biochar combined with mineral additives on (im) mobilization and (bio) availability of Pb, Cd, Cu and Zn from Pb/Zn smelter contaminated soils[J]. Ecotoxicology and Environmental Safety, 2017,145:528-538. [54] Awasthi M K, Wang Q, Chen H Y, et al. Role of compost biochar amendment on the (im) mobilization of cadmium and zinc for Chinese cabbage (Brassica rapa L.) from contaminated soil[J]. Journal of Soils and Sediments, 2019,19:3883-3897.