Citation: Dingkai Chen, Dehua Zhang, Dedong He, Jichang Lu, Liping Zhong, Caiyun Han, Yongming Luo. Relationship between oxygen species and activity/stability in heteroatom (Zr, Y)-doped cerium-based catalysts for catalytic decomposition of CH₃SH[J]. Chinese Journal of Catalysis, ;2018, 39(12): 1929-1941. doi: 10.1016/S1872-2067(18)63146-8 shu

Relationship between oxygen species and activity/stability in heteroatom (Zr, Y)-doped cerium-based catalysts for catalytic decomposition of CH₃SH

a Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, Yunnan, China;
b Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, Yunnan, China

Received Date: 29 May 2018
Revised Date: 23 July 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (21667016, 21267011, U1402233).

CeO₂,Ce_1-xZr_xO₂, and Ce_1-xY_xO_2-δ(x=0.25, 0.50, 0.75, and 1.00) have been rapidly synthesized to estimate their catalytic behavior in decomposing CH₃SH. The role of oxygen vacancies, and the relationship between the oxygen species and catalytic properties of CeO₂ andZr-doped and Y-doped ceria-based materials are investigated in detail. Combining the observed catalytic performance with the characterization results, it can be deemed that surface lattice oxygenplays a critical role in methanethiol catalytic conversion over cerium oxides. Ce_0.75Zr_0.25O₂ shows higher catalytic activity for CH₃SH decomposition due to the large amount of surface lattice oxygen,readily available oxygen species, and excellent redox properties. Ce_0.75Y_0.25O_2-δ displays better catalytic stability owing to the greater number of oxygen vacancies that would promote bulk lattice oxygen migration to the surface of the catalyst in order to replenish surface lattice oxygen. In addition, the results show that the difference in chemical valence between Ce and the heteroatoms would strongly influence the amount of surface lattice oxygen as well as the mobility of bulk-phase oxygen in these catalysts, thus affecting their activity and stability.
- Cerium-base catalyst,
- Heteroatom,
- Surface lattice oxygen,
- CH₃SH decomposition,
- Bulk oxygen migration
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Relationship between oxygen species and activity/stability in heteroatom (Zr, Y)-doped cerium-based catalysts for catalytic decomposition of CH3SH

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通讯作者: 陈斌, bchen63@163.com

Relationship between oxygen species and activity/stability in heteroatom (Zr, Y)-doped cerium-based catalysts for catalytic decomposition of CH₃SH