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三元 Ca-Mg-Al 层状双氢氧化物用于协同修复污染土壤和地下水的 As、Cd 和 Pb:特性、效果和固定化机制。

Ternary Ca-Mg-Al layered double-hydroxides for synergistic remediation of As, Cd, and Pb from both contaminated soil and groundwater: Characteristics, effectiveness, and immobilization mechanisms.

机构信息

Institute of Environment and Sustainable Development in Agriculture, Chinese Academy of Agricultural Sciences, Beijing 100081, China; Key Laboratory of Agro-Environment, Ministry of Agriculture and Rural Affairs, Institute of Environment and Sustainable Development in Agriculture, Chinese Academy of Agricultural Sciences, Beijing 100081, China.

Institute of Environment and Sustainable Development in Agriculture, Chinese Academy of Agricultural Sciences, Beijing 100081, China.

出版信息

J Hazard Mater. 2023 Jan 15;442:130030. doi: 10.1016/j.jhazmat.2022.130030. Epub 2022 Sep 20.

Abstract

Layered double hydroxides (LDH) are the cost-effective and high-efficiency materials for remediation of potentially toxic elements (PTEs) in contaminated soil and groundwater. Herein, the effectiveness and mechanisms of a ternary Ca-Mg-Al LDH (CMAL) for the synergistic remediation of As, Cd, and Pb were investigated in contaminated soils and simulative groundwaters for the first time. The immobilization efficiencies of As, Cd, and Pb in both black soil (BS) and red soil (RS) amended by CMAL at 5 wt% were all > 75%. CMAL amendment transferred more mobile As, Cd, and Pb fractions in soils to immobile species than did Ca-Al LDH and Mg-Al LDH treatments. Furthermore, using a pump-and-treat technology, 82-98% of these 3 PTEs from contaminated groundwater were successfully immobilized in both CMAL treated BS and RS top-soils. Meanwhile, leaching of Ca, Mg, and Al from CMAL was minimal indicating the material was stable. The excellent immobilization performance of CMAL for these PTEs was attributed to the coating of soil microparticles by CMAL nanosheets that allowed complexation of Ca-O-As/Cd or Mg-O-As/Cd/Pb formation, co-precipitation of Ca/Fe-As and Cd(OH), and formation of Ca-bridged ternary complex (FeO-Ca-As/Cd). The adverse effect of oppositive pH/Eh-dependence between As and Cd/Pb was overshadowed by these mechanisms and thus allowed As immobilization. Immobilization of As, Cd, and Pb by CMAL amendment was more favorable for RS soil due to its lower reduction potential and more participation of metal-(hydr)oxides for complexation. Overall, the ternary-LDH is a promising synergistic remediation strategy for multi-PTEs contaminated soil and groundwater.

摘要

层状双氢氧化物(LDH)是修复污染土壤和地下水中潜在有毒元素(PTE)的高效、经济实用的材料。本文首次研究了三元 Ca-Mg-Al LDH(CMAL)在污染土壤和模拟地下水中对 As、Cd 和 Pb 的协同修复效果及其作用机制。在 5wt%的用量下,CMAL 对黑土(BS)和红土(RS)的固定效率均>75%,对 As、Cd 和 Pb 的固定效率均>75%。CMAL 改性使土壤中更多的可移动 As、Cd 和 Pb 形态转化为不可移动形态,优于 Ca-Al LDH 和 Mg-Al LDH 处理。此外,采用泵送处理技术,82-98%的污染地下水中的这 3 种 PTE 成功地固定在 CMAL 处理的 BS 和 RS 表土中。同时,CMAL 中的 Ca、Mg 和 Al 的浸出量很小,表明材料稳定。CMAL 对这些 PTE 的优异固定性能归因于 CMAL 纳米片对土壤微粒的包覆,允许 Ca-O-As/Cd 或 Mg-O-As/Cd/Pb 的络合、Ca/Fe-As 和 Cd(OH)的共沉淀以及 Ca 桥接三元配合物(FeO-Ca-As/Cd)的形成。相反,As 和 Cd/Pb 的 pH/Eh 依赖性之间的不利影响被这些机制所掩盖,从而允许 As 的固定。由于还原电位较低且金属-(水)氧化物参与络合的程度较高,CMAL 改性对 RS 土壤中 As、Cd 和 Pb 的固定更为有利。总的来说,三元-LDH 是一种很有前途的协同修复多 PTE 污染土壤和地下水的策略。

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