Chinese Journal of Catalysis ›› 2020, Vol. 41 ›› Issue (12): 1846-1854.DOI: 10.1016/S1872-2067(20)63635-X

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Mechanochemical redox-based synthesis of highly porous CoxMn1-xOy catalysts for total oxidation

Jiafeng Baoa, Hao Chenb, Shize Yangc, Pengfei Zhanga   

  1. 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:2020-03-21 Revised:2020-04-23 Online:2020-12-18 Published:2020-08-14
  • Supported by:
    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.

Abstract: A mechanochemical redox reaction between KMnO4 and CoCl2 was developed to obtain a CoxMn1-xOy 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 CoxMn1-xOy 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 CoxMn1-xOy 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 CoxMn1-xOy 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 CoxMn1-xOy catalyst (1 kg) can be achieved via ball milling, which may provide a potential strategy for real world catalysis.

Key words: Mechanochemical synthesis, Solid-state synthesis, Porous metal oxide, CoxMn1-xOy catalyst, Hydrocarbon combustion