Citation: Jiafeng Bao, Hao Chen, Shize Yang, Pengfei Zhang. Mechanochemical redox-based synthesis of highly porous Co_xMn_1-xO_y catalysts for total oxidation[J]. Chinese Journal of Catalysis, ;2020, 41(12): 1846-1854. doi: 10.1016/S1872-2067(20)63635-X shu

Mechanochemical redox-based synthesis of highly porous Co_xMn_1-xO_y catalysts for total oxidation

a School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;
b Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, USA;
c Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY11973, USA

Received Date: 21 March 2020
Revised Date: 23 April 2020

Fund Project: This work was supported by the National Natural Science Foundation of China (21776174), the Open Foundation of the State Key Laboratory of Ocean Engineering (Shanghai Jiao Tong University of China) (1809), Shanghai Jiao Tong University Scientific and Technological Innovation Funds (2019QYB06), China Shipbuilding Industry Corporation (CSIC) and Zhejiang XinAn Chemical Industry Corporation.

A mechanochemical redox reaction between KMnO₄ and CoCl₂ was developed to obtain a Co_xMn_1-xO_y catalyst with a specific surface area of 479 m² g^-1, which was higher than that obtained using a co-precipitation (CP) method (34 m² g^-1), sol-gel (SG) method (72 m² g^-1), or solution redox process (131 m² g^-1). During catalytic combustion, this Co_xMn_1-xO_y catalyst exhibited better activity (T₁₀₀ for propylene= ~200 ℃) than the control catalysts obtained using the SG (325 ℃) or CP (450 ℃) methods. The mechanical action, mainly in the form of kinetic energy and frictional heating, may generate a high degree of interstitial porosity, while the redox reaction could contribute to good dispersion of cobalt and manganese species. Moreover, the as-prepared Co_xMn_1-xO_y catalyst worked well in the presence of water vapor (H₂O 4.2%, >60 h) or SO₂ (100 ppm) and at high temperature (400 ℃, >60 h). The structure MnO₂·(CoOOH)_2.93 was suggested for the current Co_xMn_1-xO_y catalyst. This catalyst could be extended to the total oxidation of other typical hydrocarbons (T₉₀=150 ℃ for ethanol, T₉₀ =225 ℃ for acetone, T₉₀=250 ℃ for toluene, T₉₀ =120 ℃ for CO, and T₉₀=540 ℃ for CH₄). Scale-up of the synthesis of Co_xMn_1-xO_y catalyst (1 kg) can be achieved via ball milling, which may provide a potential strategy for real world catalysis.
- Mechanochemical synthesis,
- Solid-state synthesis,
- Porous metal oxide,
- Co_xMn_1-xO_y catalyst,
- Hydrocarbon combustion
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Mechanochemical redox-based synthesis of highly porous CoxMn1-xOy catalysts for total oxidation

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通讯作者: 陈斌, bchen63@163.com

Mechanochemical redox-based synthesis of highly porous Co_xMn_1-xO_y catalysts for total oxidation