New Tricks for an Old Dog: Grubbs Catalysts Enable Efficient Hydrogen Production from Aqueous-Phase Methanol Reforming

Qian Wang, Jialing Lan, Rong Liang, Yihao Xia, Lei Qin, Lung Wa Chung, Zhiping Zheng

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Herein, we report a new application of the prize-winning Grubbs catalysts, which have been widely applied for olefin metathesis, for hydrogen production from aqueous-phase methanol reforming under easily achievable conditions (1 atm, <100 °C) with negligible CO formation. Out of the catalysts tested, the best turnover frequency (158 h-1) and turnover number (11424, 72 h) were both achieved with a third-generation Grubbs catalyst (G-III). The best TOF was achieved with G-III and is competitive when compared with some of the best results reported ( Chem. Rev. 2018, 118, 372−433). Also, G-III is found to be a versatile catalyst for the dehydrogenation of ethanol and formic acid. Mechanistic studies and DFT calculations shed light on the reaction mechanism, which involves an unusual substrate (solvent)-assisted six-membered-ring (σ-bond) metathesis pathway. This work should open up new opportunities in catalyst design in connection with the hydrogen economy and, more generally, with the development of clean and renewable energies.

Original languageEnglish (US)
Pages (from-to)2212-2222
Number of pages11
JournalACS Catalysis
Volume12
Issue number4
DOIs
StatePublished - Feb 18 2022
Externally publishedYes

Keywords

  • DFT
  • Grubbs Catalysts
  • Hydrogen Economy
  • Methanol
  • dehydrogenation

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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