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Antimony immobilization mechanism on schwertmannite: Insights from the microstructure of schwertmannite

斯沃特曼矿 化学 吸附 吸附 齿合度 硫酸盐 无机化学 金属 物理化学 有机化学 针铁矿
作者
Jun Shan,Mengchang He,Peng Liu,Wenting Wang,Chunye Lin,Wei Ouyang,Xitao Liu,Jianwei Zhou,Haijiao Xie
出处
期刊:Geochimica et Cosmochimica Acta [Elsevier BV]
卷期号:359: 71-83 被引量:5
标识
DOI:10.1016/j.gca.2023.09.005
摘要

Schwertmannite affects the mobility of antimony (Sb) in acid mine drainage, yet the Sb sorption mechanism remains elusive. In this study, the molecular-level mechanism and the driving force of Sb(V) immobilized on schwertmannite were investigated by a combination of wet chemistry, extended X-ray absorption fine structure (EXAFS) analysis, density functional theory (DFT) calculations, and a surface complexation model (SCM). The observed sorption capacity for Sb(V) was as high as 235.63 mg/g. Such remarkable sorption capacity is primarily achieved by the anion exchange reaction and surface complexation reaction of Sb(V) with sulfate and surface/tunnel inner-surface hydroxyl groups, respectively, and the contribution of the anion exchange reaction to Sb(V) immobilization decreases markedly with increasing Sb(V) loading or pH. The loading of Sb(V) appears to be the key parameter controlling its immobilization mechanism on schwertmannite. Low-loaded Sb(V) primarily generates bidentate-mononuclear and bidentate-binuclear surface complexes (adsorption products) and is concurrently partly incorporated into the Fe-O framework of schwertmannite to form a hexadentate-hexanuclear complex (incorporation product). With increasing Sb(V) loading, Sb is primarily adsorbed on the surface and in the tunnel of schwertmannite with the formation of bidentate-mononuclear (dominant) and bidentate-binuclear complexes without incorporation. The inconsistency of the immobilization mechanism is controlled by the amount of released sulfate induced by Sb(V). The substantial system energy reduction caused by the formation of Sb(V) adsorption and incorporation products on the surface and in the tunnel of schwertmannite is the driving force for the stable immobilization of Sb(V) by schwertmannite, and the energy reduction caused by tunnel complexes is far more obvious than that caused by surface complexes. A charge distribution multisite complexation model was established based on bidentate-mononuclear and bidentate-binuclear surface complexes with fitted Log K values of 21.99±0.18 and 12.84±0.92, respectively, which consistently predicted Sb(V) sorption across pH 3.0-9.0 for all involved Sb(V) loadings. In addition, Sb(V) has a strong stabilizing effect on the schwertmannite structure and broadens its pH stability window (pH 3.0-9.0). This study facilitates elucidation of the fate and geochemical cycling of Sb in the mining environment and helps to promote the application of the microstructure of schwertmannite in other studies of microscopic interface chemistry.
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