吸附剂
砷
吸附
化学
化学吸附
催化作用
锰
无机化学
催化氧化
化学工程
有机化学
工程类
作者
Yue Zhang,Bangcheng Zhao,Caijie Wang,Yuyu Huang,Xiang Liu,Ruikun Wang,Chunbo Wang
标识
DOI:10.1016/j.jhazmat.2023.132079
摘要
Arsenic oxidation plays a crucial role in its removal, which has been identified in numerous studies. However, the mechanisms, especially reaction pathways of arsenic oxidation on sorbent surfaces remain inadequately explored. In this work, the effects of Mn doping on arsenic adsorption and oxidation were first verified by adsorption experiments. Subsequently, DFT calculations were carried out to identify alterations in the adsorption energies, active sites, and oxidation pathways. By integrating the experimental and simulation results, a dual-functional framework encompassing adsorption and catalysis of Mn-modified Fe-based material was distinctly established. For adsorption, the introduction of manganese into iron-based sorbent considerably enhanced As2O3 adsorption owing to the increased active sites available for As2O3 chemisorption and the promotion of surface nucleophilicity. Concerning oxidative catalysis, the incorporation of MnO2 augmented surface catalytic oxidation and provided a substantial amount of active Oload. Consequently, the arsenic oxidation occurring on the Mn-modified sorbent surfaces possessed a lower oxidation RDS energy barrier and a shorter oxidation pathway than those on the bare sorbent surfaces. These experimental and simulation results provide a theoretical basis for the design and application of efficient gaseous arsenic adsorbents.
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