Citation: Panpan Wang, Jiahao Duan, Jie Wang, Fuming Mei, Peng Liu. Elucidating structure-performance correlations in gas-phase selective ethanol oxidation and CO oxidation over metal-doped γ-MnO₂[J]. Chinese Journal of Catalysis, ;2020, 41(8): 1298-1310. doi: 10.1016/S1872-2067(20)63551-3 shu

Elucidating structure-performance correlations in gas-phase selective ethanol oxidation and CO oxidation over metal-doped γ-MnO₂

Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China

Received Date: 3 December 2019
Revised Date: 25 December 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21673088, 21972050).

Despite of considerable efforts on the MnO₂-based catalytic combustion, the different structural and component requirements of MnO₂ for gas-phase selective oxidation and complete oxidation largely remain unknown. By comparing four types of MnO₂ with different crystal structures (α, β, γ and δ), γ-MnO₂ was found to be the most efficient catalyst for both aerobic selective oxidation of ethanol and CO oxidation. The structural effect of γ-MnO₂ was further investigated by doping metal ions into the framework and by comparing the catalytic performance in the gas-phase aerobic oxidation of CO and ethanol. Among ten M-γ-MnO₂ catalysts, Zn-γ-MnO₂ showed the lowest temperature (160℃) for achieving 90% CO conversion. The CO oxidation activity of the M-γ-MnO₂ catalysts was found to be more relevant to the surface acidity-basicity than the reducibility. In contrast, surface reducibility has been demonstrated to be more crucial in the gas-phase ethanol oxidation. Cu-γ-MnO₂ with higher reducibility and more oxygen vacancies of Mn²⁺/Mn³⁺ species exhibited higher catalytic activity in the selective ethanol oxidation. Cu-γ-MnO₂ achieved the highest acetaldehyde yield (75%) and space-time-yield (5.4 g g_cat^-1 h^-1) at 200℃, which are even comparable to the results obtained by the state-of-the-art silver and gold-containing catalysts. Characterization results and kinetic studies further suggest that the CO oxidation follows the lattice oxygen-based Mars-van Krevelen mechanism, whereas both surface lattice oxygen and adsorbed oxygen species involve in the ethanol activation.
- MnO₂,
- Metal doping,
- Ethanol oxidation,
- Acetaldehyde,
- Catalytic CO oxidation
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Elucidating structure-performance correlations in gas-phase selective ethanol oxidation and CO oxidation over metal-doped γ-MnO2

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通讯作者: 陈斌, bchen63@163.com

Elucidating structure-performance correlations in gas-phase selective ethanol oxidation and CO oxidation over metal-doped γ-MnO₂