Surface Complex and Nonradical Pathways Contributing to High-Efficiency Degradation of Perfluorooctanoic Acid on Oxygen-Deficient In2O3 Derived from an In-Based Metal Organic Framework

全氟辛酸 吸附 降级(电信) 化学吸附 氧气 傅里叶变换红外光谱 化学 无机化学 环境化学 化学工程 物理化学 计算机科学 有机化学 电信 工程类
作者
Xin Gao,Juan Chen,Huinan Che,Yanhui Ao,Peifang Wang
出处
期刊:ACS ES&T water [American Chemical Society]
卷期号:2 (8): 1344-1352 被引量:21
标识
DOI:10.1021/acsestwater.2c00078
摘要

The mediating role of surface structure of In2O3 on the adsorption and photocatalytic degradation of perfluorooctanoic acid (PFOA) is important but still unclear. Herein, In2O3 with various oxygen vacancy concentrations are designed by pyrolyzing a metal organic framework (MIL-68(In)-NH2) for PFOA degradation. The results demonstrate that the In2O3-400 obtained at a lower pyrolysis temperature of 400 °C possesses the highest oxygen vacancy concentration, thus exhibiting remarkably boosted adsorption capacity and degradation performance for PFOA. Adsorption kinetics, isotherm adsorption model, and Fourier transform infrared spectroscopy (FTIR) results show that PFOA is chemically adsorbed on the In2O3-400 surface in the form of monodentate mode. Notably, there is a linear correlation between the adsorption capacity and the degradation kinetic rate constant of In2O3-400 for PFOA, indicating that surface adsorption is a prerequisite for the PFOA degradation. Furthermore, density functional theory (DFT) results indicate that oxygen vacancies, as the structural characteristic for PFOA chemisorption, can promote the nonradical oxidation process of PFOA. This study provides a new perspective to explain the role of the surface structure of In2O3 in relation to its adsorption and photocatalytic performance for PFOA, which is helpful for the development of more effective PFOA adsorption coupled degradation technology.
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