Citation: Pengwei Wang, Xin Zhang, Guofeng Zhao, Ye Liu, Yong Lu. Oxidative coupling of methane: MO_x-modified (M=Ti, Mg, Ga, Zr) Mn₂O₃-Na₂WO₄/SiO₂ catalysts and effect of MO_x modification[J]. Chinese Journal of Catalysis, ;2018, 39(8): 1395-1402. doi: 10.1016/S1872-2067(18)63076-1 shu

Oxidative coupling of methane: MO_x-modified (M=Ti, Mg, Ga, Zr) Mn₂O₃-Na₂WO₄/SiO₂ catalysts and effect of MO_x modification

Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China

Received Date: 22 February 2018
Revised Date: 31 March 2018

Fund Project: This work was supported by the Basic Key Project (18JC1412100) from the Shanghai Municipal Science and Technology Commission, the National Natural Science Foundation of China (21773069, 21703069, 21473057, U1462129), and the National Basic Research Program of China (973 program, 2011CB201403) from the MOST of China.

Mn₂O₃-Na₂WO₄/SiO₂ is considered as the most promising catalyst for the oxidative coupling of methane (OCM) process; however, it only has a better catalytic performance over 800℃. To improve its low-temperature performance, an attempt has been made to modify the Mn₂O₃-Na₂WO₄/SiO₂ catalyst using TiO₂, MgO, Ga₂O₃, and ZrO₂. Among the synthesized catalysts, the TiO₂-modified Mn₂O₃-Na₂WO₄/SiO₂ catalyst shows markedly improved low-temperature OCM performance, achieving a high CH₄ conversion of ~23% and a good C₂-C₃ selectivity of ~73% at 700℃ (the catalyst bed temperature), along with promising stability for at least 300 h without signs of deactivation. In comparison with the unmodified Mn₂O₃-Na₂WO₄/SiO₂ catalyst, the TiO₂ modification results in significant improvement in the low-temperature activity/selectivity, whereas the MgO modification has almost no impact and the Ga₂O₃ and ZrO₂ modifications have a negative effect. The X-ray diffraction (XRD) and Raman results reveal that the formation of a MnTiO₃ phase and a MnTiO₃-dominated catalyst surface is crucial for the improvement of the low-temperature activity/selectivity in the OCM process.
- Oxidative coupling of methane,
- Light olefins,
- Ethylene,
- Oxide modification,
- MnTiO₃
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Oxidative coupling of methane: MOx-modified (M=Ti, Mg, Ga, Zr) Mn2O3-Na2WO4/SiO2 catalysts and effect of MOx modification

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Oxidative coupling of methane: MO_x-modified (M=Ti, Mg, Ga, Zr) Mn₂O₃-Na₂WO₄/SiO₂ catalysts and effect of MO_x modification