4.6 Article

Reaction Mechanism for Methane-to-Methanol in Cu-SSZ-13: First-Principles Study of the Z2[Cu2O] and Z2[Cu2OH] Motifs

期刊

CATALYSTS
卷 11, 期 1, 页码 -

出版社

MDPI
DOI: 10.3390/catal11010017

关键词

DFT; reaction mechanism; micro-kinetic model; small-pore zeolite; chabazite; SSZ-13; copper; methane-to-methanol; direct conversion

资金

  1. Knut and AliceWallenberg Foundation through the project Atomistic design of catalysts [KAW2015.0058]
  2. Competence Centre for Catalysis (KCK) at Chalmers University of Technology
  3. Chalmers University of Technology
  4. Swedish Energy Agency
  5. AB Volvo
  6. ECAPS AB
  7. Johnson Matthey AB
  8. Preem AB
  9. Scania CV AB
  10. Umicore Denmark ApS
  11. SNIC grant

向作者/读者索取更多资源

Research on the partial oxidation of methane over small-pore copper-exchanged zeolite SSZ-13 shows that the Z2[Cu2O] motif has an exergonic reaction path, but micro-kinetic modeling indicates that neither Z2[Cu2O] nor Z2[Cu2OH] are notably active under the reaction conditions. These findings emphasize the importance of the detailed structure of the active site in catalytic reactions.
As transportation continues to increase world-wide, there is a need for more efficient utilization of fossil fuel. One possibility is direct conversion of the solution gas bi-product CH4 into an energy-rich, easily usable liquid fuel such as CH3OH. However, new catalytic materials to facilitate the methane-to-methanol reaction are needed. Using density functional calculations, the partial oxidation of methane is investigated over the small-pore copper-exchanged zeolite SSZ-13. The reaction pathway is identified and the energy landscape elucidated over the proposed motifs Z2[Cu2O] and Z2[Cu2OH]. It is shown that the Z2[Cu2O] motif has an exergonic reaction path, provided water is added as a solvent for the desorption step. However, a micro-kinetic model shows that neither Z2[Cu2O] nor Z2[Cu2OH] has any notable activity under the reaction conditions. These findings highlight the importance of the detailed structure of the active site and that the most stable motif is not necessarily the most active.

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