期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 305, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.121019
关键词
Multi-shelled hollow microspheres; Cobalt oxide; Peroxymonosulfate activation; Catalytic selectivity
资金
- National Key Research and Development Program of China [2019YFD1100104-03-01]
- National Natural Science Foundation of China [52000048]
- Cooperative Researching Project of Chunhui Program, Ministry of Education, China [HLJ2019006]
- Postdoctoral Science Foundation Grant, China [2020T130152]
- Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology [QA202008]
A multi-shelled hollow micro-reactor with tunable shell number, thickness and porosity was constructed using nanosized Co3O4 for the catalysis of PMS. Triple-shelled hollow microspheres showed superior catalytic activity and selectivity could be optimized by adjusting shell thickness and porosity.
Herein, a multi-shelled hollow micro-reactor with tunable shell number, thickness and porosity is constructed by nanosized Co3O4 to catalyze peroxymonosulfate (PMS) for the first time. Triple-shelled hollow microspheres (TS HM) exhibit superior catalytic activity with the degradation rate of 0.4158 min(-1), which is 22, 5.8, 1.9 times of that of solid nanoparticles, quadruple-shelled hollow microspheres (QS-HM), and double-shelled hollow microspheres (DS-HM), respectively. Such an outstanding performance of TS-HM is attributed to more exposed active sites, strong capacity of Co-II regeneration and desired structure stability. Furthermore, the selectivity of 2-cholorophenol (2-CP) over humic acid (HA) is optimized by tuning shell thickness and porosity. The thick shell and narrow pore size are recognized as the dominant contributors based on size exclusion effects. Significantly, mechanistic studies reveal that O-2(.-) is generated on the catalyst surface via O-2 adsorption and reduction by oxygen vacancies, and plays an important role for Co-II regeneration.
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