期刊
APPLIED SURFACE SCIENCE
卷 579, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apsusc.2021.151978
关键词
Mn3O4; Cd0.9Zn0.1S; Photothermal catalysis; Aromatic alcohol; Selective oxidation
类别
资金
- National Natural Science Foundation of China (NSFC) [51772118, 51972134, 52002142]
- University Natural Science Research Project of Anhui Province [KJ2019A0602]
- fund of the State Key Laboratory of Catalysis in DICP [N-20-09, N-20-10]
The Mn3O4/CZS photothermal catalysts show enhanced catalytic performance for the selective oxidation of aromatic alcohol, with high selectivity and yield. This study proposes a photo-thermal synergetic catalytic mechanism for the efficient selective oxidation of aromatic alcohol.
Constructing photothermal catalysts is a promising strategy to improve the efficiency of selective photocatalytic oxidation of aromatic alcohol to aromatic aldehyde. Herein, Mn3O4/Cd0.9Zn0.1S (CZS) photothermal catalysts have been prepared by introducing an as-prepared CZS photocatalyst during Mn3O4 preparation. The Mn3O4/ CZS samples exhibit higher catalytic performance for selective oxidation (SO) of aromatic alcohol. Especially, the optimized 10% Mn3O4/CZS sample possesses 7 times yield of CZS with an over 90% selectivity. The photo-thermal synergetic catalytic mechanism of Mn3O4/CZS for the SO of aromatic alcohol was proposed. Mn3O4(2MnO center dot MnO2) severs as the center of thermal catalysis and O-2 adsorption. The high-valent MnO2 oxidized aromatic alcohols into aromatic aldehydes and the generated low-valent MnO was oxidized to MnO2 by adsorbed O-2, forming a thermal cycling reaction. Meanwhile, the photoexcited electrons (e(-)) originating from CZS were transferred to Mn(3)O(4 )due to the matching energy level of MnO and CZS and further reduced the adsorbed O-2 to active oxygen (center dot O-2(-)) and lattice oxygen (O-2(-)), availably accelerating the separation of photoexcited carriers. Finally, center dot O-2(-), O2- and photoexcited holes (h(+)) can also selectively oxidize aromatic alcohol. This study provides an alternative paradigm for the efficient SO of aromatic alcohol.
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