Highly Selective Oxidation of Methane into Methanol over Cu-Promoted Monomeric Fe/ZSM-5

Tao Yu, Zhi Li, Lu Lin, Shengqi Chu, Yang Su, Weiyu Song, Aiqin Wang, Bert M. Weckhuysen, Wenhao Luo*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

The selective oxidation of methane into methanol is of paramount importance but poses significant challenges in achieving high methanol productivity and selectivity, especially under mild reaction conditions. We show that a Cu-modified monomeric Fe/ZSM-5 catalyst is a highly efficient material for the direct conversion of methane into methanol in the liquid phase using H2O2 as an oxidant at low temperatures, which exhibits an excellent methanol productivity of 431 molMeOH·mol-1Fe·h-1 (with a methanol selectivity of μ80% over the Cu-Fe(2/0.1)/ZSM-5 catalyst). Combining the control experiments and comprehensive characterization results by among others, Mössbauer spectroscopy, and electron paramagnetic resonance as well as density functional theory calculations, we found that Cu species in the Cu-Fe(2/0.1)/ZSM-5 catalyst play a pivotal role in facilitating the formation of •OH radicals, which quickly react with •CH3 radicals to form CH3OH. These findings provide valuable insights into the rational design of metal-zeolite combinations for the selective oxidation of methane into methanol.

Original languageEnglish
Pages (from-to)6684-6691
Number of pages8
JournalACS Catalysis
Volume11
Issue number11
DOIs
Publication statusPublished - 4 Jun 2021

Bibliographical note

Funding Information:
Financial support for this work comes from the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020100) and the Foundation of Dalian Institute of Chemical Physics (DICP I201915), which is gratefully acknowledged. We are also grateful for the support for X-ray absorption spectroscopy experiments from the Beijing Synchrotron Radiation Facility (BSRF).

Publisher Copyright:
© 2021 American Chemical Society.

Funding

Financial support for this work comes from the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020100) and the Foundation of Dalian Institute of Chemical Physics (DICP I201915), which is gratefully acknowledged. We are also grateful for the support for X-ray absorption spectroscopy experiments from the Beijing Synchrotron Radiation Facility (BSRF).

Keywords

  • characterization
  • copper
  • methane
  • monomeric Fe species
  • zeolite

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