Selective catalytic activation of peroxymonocarbonate over a Co/Al2O3 catalyst

被引:6
|
作者
Zhou, Yi [1 ,2 ]
Yane, Zihan [1 ,2 ]
Jiang, Yiqian [1 ,2 ]
Shen, Zihan [1 ,2 ]
Zhao, Peiqing [1 ]
Meng, Xu [1 ]
机构
[1] Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
关键词
Peroxymonocarbonate; Catalytic activation; Oxygen vacancy; Lewis acid site; Advanced oxidation processes; INITIO MOLECULAR-DYNAMICS; HYDROGEN-PEROXIDE; EFFICIENT DEGRADATION; HETEROGENEOUS ACTIVATION; BICARBONATE ACTIVATION; ADVANCED OXIDATION; OXYGEN; CO3O4; MECHANISM; WATER;
D O I
10.1016/j.apcatb.2024.124748
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We assessed the selective catalytic performance of Co/Al2O3 in activating HCO4- for tetracycline degradation by studying the activation of oxidants and the generation of reactive oxygen species. Co/Al2O3 exhibited high catalytic selectivity towards HCO4- in the presence of H2O2, achieving a H2O2 utilization efficiency of 74.9 % for the production of center dot OH. The Co/Al2O3-catalyzed HCO4--based system oxidized 89.2 % of tetracycline primarily through center dot OH and CO3 center dot- generated from HCO4- activation, while center dot O-2 and O-1(2) played minor roles in degradation. Low-valent cobalt species served as catalytic active sites for HCO4- activation. Abundant oxygen vacancies on Co/Al2O3 accelerated the electron transfer, forming a local electron-rich region that preferentially adsorbed electrophilic HCO4- and provided additional active sites for HCO4- activation. Furthermore, the increased Lewis acid sites assisted HCO4- activation by stabilizing the leaving carbonate groups. This work offers insights into the structure-activity relations of catalysts for the selective catalytic activation of HCO4-.
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页数:12
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