Identification of the active sites and mechanism for partial methane oxidation to methanol over copper-exchanged CHA zeolites

Yu Mao, P. Hu*

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

To make methane a suitable energy carrier and transport less costly, it is an urgent and challenging task for us to convert methane to liquid under mild conditions efficiently. In this study, we explored partial methane oxidation to methanol by density functional theory (DFT) calculations using a hybrid functional (HSE06) with van der Waals (vdW) interactions. The stabilities of different active sites over SSZ-13 and SAPO-34, two CHA type zeolites, are thoroughly investigated by ab initio molecular dynamics (AIMD) simulations and ab initio thermodynamics analyses. Four possible active sites, namely [CuOHCu]2+, [Cu(OH)2Cu]2+, [CuOCu]2+ and [CuOH]+, are identified stable. Methane-to-methanol reaction mechanisms are further studied upon these most stable active sites, among which [CuOCu]2+ and [CuOH]+ are proved to be reactive. The migration of species among zeolite pores are also discussed, which accounts for the activity on [CuOH]+ sites. This concept may represent a more complete picture of catalytic reactions over zeolites in general.

Original languageEnglish
Pages (from-to)850-859
Number of pages10
JournalScience China Chemistry
Volume63
Issue number6
Early online date25 Mar 2020
DOIs
Publication statusPublished - 01 Jun 2020

Keywords

  • CHA zeolites
  • DFT
  • heterogeneous catalysis
  • methane-to-methanol

ASJC Scopus subject areas

  • Chemistry(all)

Fingerprint Dive into the research topics of 'Identification of the active sites and mechanism for partial methane oxidation to methanol over copper-exchanged CHA zeolites'. Together they form a unique fingerprint.

Cite this