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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
来源:
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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