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 language | English (US) |
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Pages (from-to) | 2212-2222 |
Number of pages | 11 |
Journal | ACS Catalysis |
Volume | 12 |
Issue number | 4 |
DOIs | |
State | Published - Feb 18 2022 |
Externally published | Yes |
Keywords
- DFT
- Grubbs Catalysts
- Hydrogen Economy
- Methanol
- dehydrogenation
ASJC Scopus subject areas
- Catalysis
- General Chemistry