催化作用
化学
钙钛矿(结构)
锰
吸附
氧化还原
氧气
氧化物
反应速率常数
无机化学
动力学
物理化学
结晶学
有机化学
物理
量子力学
作者
Yu Dan,Jiahong He,Taiping Xie,Jun Yang,Jiankang Wang,Jinchen Xie,Huiting Shi,Zongyu Gao,Bing Xiang,Dionysios D. Dionysiou
标识
DOI:10.1016/j.jhazmat.2022.130085
摘要
Material-enhanced heterogeneous peroxymonosulfate (PMS) activation for degradation of antibiotic in water has attracted intensive attention. However, one challenge is the electron transfer efficiency from the material to PMS for reactive oxygen species (ROS) production. Considering that the B-sites of perovskite oxides are closely associated with the catalytic performance, partial substitution of the B-sites of perovskite oxides can enhance the redox cycle of metals. Consequently, adjusting the ratio of each element at the B site can introduce oxygen vacancies on the surface of perovskite. Herein, a method was developed in which manganese (Mn) partially substitutes B-sites to modify surface properties of SrCoO2.52 perovskite oxides, resulting in the enhancement of catalytic activity. In degradation kinetics studies using SrCoMnO3-δ-0.5/PMS (SrCoMnO3-δ-0.5 denotes that the molar substitution of Mn at the B site of SrCoO2.52 perovskite oxide is 0.5) reaction system and sulfamethoxazole (SMX) as the target pollutant, it was found that the reaction rate constant (kobs) is 0.287 min-1 which is 2.4 times that of SrCoO2.52/PMS system. Experimental and theoretical analyses revealed that Mn-O covalent bonding governs the intrinsic catalytic activity of SrCoMnO3-δ-0.5 perovskite oxides. The Mn sites exhibits stronger adsorption energy with PMS than the Co sites, facilitating the breaking of O-O bond. Simultaneously, oxygen vacancies and surface adsorbed oxygen species have a synergistic effect for PMS adsorption. This work can provide a potential route in developing advanced catalysts based on manipulation of the B-sites of perovskite oxides for PMS activation.
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