Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 540-558.DOI: 10.19894/j.issn.1000-0518.210461

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Recent Advances in Direct Oxidation of Methane to Methanol

Ke WANG, Xiao WANG(), Shu-Yan SONG   

  1. State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China
  • Received:2021-09-10 Accepted:2021-12-10 Published:2022-04-01 Online:2022-04-19
  • Contact: Xiao WANG
  • About author:skybyyn@ciac.ac.cn
  • Supported by:
    the National Natural Science Foundation of China(21771173);the National Key Research and Development Program of China(2016YFA0203200)

Abstract:

The methods for synthesizing methanol from methane include indirect method and direct catalytic oxidation method, but the indirect method requires high equipment, and the methane conversion rate and methanol selectivity are not ideal. Direct catalytic oxidation method (DMTM) can produce methanol with high selectivity through a one-step reaction, and has huge application potential. For DMTM, the homogeneous catalytic system usually requires a special reaction medium combined with a precious metal catalyst. Although the reaction efficiency is high, it is corrosive to the reaction equipment, the product is not easy to separate, and the application prospect is poor. Liquid phase-heterogeneous catalysis generally uses H2O2 as the oxidant, Au, Pd, Fe, Cu and other metal elements as the main active component of the catalyst, and·OH is the main oxidation active substance, which can be used at low temperature to realize the activation and oxidation of methane. Therefore, heterogeneous catalytic systems are currently the mainstream of research. Gas phase-heterogeneous catalysis mainly uses O2 and N2O as oxidants. The former is more active, and the latter is more selective for products. In addition, H2O in anaerobic systems can also be directly used as oxygen donors, commonly Cu, Fe, Rh, etc. elements are used as catalysts. Zeolite molecular sieves are the most widely used support, and metal oxides, metal organic frameworks (MOFs) and graphene are also involved. Multi-metal synergistic catalysis has achieved good results. This article mainly summarizes the research on the direct catalytic oxidation of thermally catalyzed methane to methanol in recent years, and prospects for future research directions.

Key words: Homogeneous catalysis, Heterogeneous catalysis, Gas phase-heterogeneous catalysis, Liquid phase-heterogeneous catalysis, CH4 oxidation

CLC Number: