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砷酸根(Ⅴ)在不同条件下形成的天然次生铁矿物上的吸附:吸附行为与表面结构的关系。

Sorption of arsenate(Ⅴ) to naturally occurring secondary iron minerals formed at different conditions: The relationship between sorption behavior and surface structure.

机构信息

Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, School of Environmental Science and Engineering, Guangzhou University, Guangzhou, 510006, China.

Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, School of Environmental Science and Engineering, Guangzhou University, Guangzhou, 510006, China.

出版信息

Chemosphere. 2021 Dec;285:131525. doi: 10.1016/j.chemosphere.2021.131525. Epub 2021 Jul 10.

DOI:10.1016/j.chemosphere.2021.131525
PMID:34265703
Abstract

Arsenic (As) is a problematic pollutant that can cause cancer and other chronic diseases due to its potential toxicity. Iron (oxyhydr)oxides can readily sorb As and play important roles in the geochemical cycle of As. Attention has mainly been given to the affinity and mechanism of As sorption by synthetic pure iron (oxyhydr)oxides, and little is known about the relationship between As behavior and multicomponent secondary iron minerals (SIMs) naturally formed in acid mine drainage (AMD). To investigate this relationship, we performed sorption kinetics, isotherm and competitive sorption experiments to investigate As(V) sorption behaviors on naturally formed SIMs harvested from different runoff zones of an abandoned coal mine. Several spectroscopic analyses were used to evaluate the structural and component changes and phase transformation. Three environmental SIMs formed at nascent (n-SIM), transient (t-SIM) and mature (m-SIM) stages were determined to be similar in the element components of Fe, S and O but different in structure. As(V) sorption behaviors on these environmental SIMs followed a pseudo-second-order kinetic model, and the sorption extent followed the sequence of n-SIM > t-SIM > m-SIM. As(V) sorption is not significantly influenced by Na/Ca concentration or ionic strength except for that of PO, and it slightly decreases as the Cr(Ⅲ) concentration increases but increases with increasing Sb(Ⅲ)/(V) concentration. The results of spectral analyses indicate that As(V) immobilization mainly depends on exchange with SO and surface complexation, along with the phase transformation of schwertmannite/jarosite to goethite and other phases. These findings are helpful for better understanding the geochemical behaviors of As(V) associated with environmental SIMs.

摘要

砷(As)是一种有问题的污染物,由于其潜在的毒性,可能会导致癌症和其他慢性疾病。铁(氧)氢氧化物可以很容易地吸附砷,并在砷的地球化学循环中发挥重要作用。人们主要关注合成纯铁(氧)氢氧化物对砷的吸附亲和力和机制,而对于在酸性矿山排水(AMD)中自然形成的多组分次生铁矿物(SIMs)中砷的行为与 SIMs 的关系知之甚少。为了研究这种关系,我们进行了吸附动力学、等温线和竞争吸附实验,以研究从废弃煤矿不同径流区采集的自然形成的 SIM 对砷(V)的吸附行为。使用几种光谱分析来评估结构和成分变化以及相转变。确定在初生(n-SIM)、瞬态(t-SIM)和成熟(m-SIM)阶段形成的三种环境 SIM 在 Fe、S 和 O 的元素成分上相似,但结构不同。这些环境 SIM 对砷(V)的吸附行为符合准二级动力学模型,吸附程度的顺序为 n-SIM>t-SIM>m-SIM。除了 PO 之外,Na/Ca 浓度或离子强度对 As(V) 的吸附没有显著影响,Cr(Ⅲ)浓度略有增加但 Sb(Ⅲ)/(V)浓度增加时略有减少。光谱分析结果表明,As(V)的固定主要取决于与 SO 的交换和表面络合,以及水铁矿/黄钾铁矾向针铁矿和其他相的转变。这些发现有助于更好地理解与环境 SIMs 相关的 As(V)的地球化学行为。

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