@article{e760a934a39d49b3b26bc70d6b01c460,
title = "New Tricks for an Old Dog: Grubbs Catalysts Enable Efficient Hydrogen Production from Aqueous-Phase Methanol Reforming",
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.",
keywords = "DFT, Grubbs Catalysts, Hydrogen Economy, Methanol, dehydrogenation",
author = "Qian Wang and Jialing Lan and Rong Liang and Yihao Xia and Lei Qin and Chung, {Lung Wa} and Zhiping Zheng",
note = "Funding Information: Financial support by National Natural Science Foundation of China (21933003, 22193020, and 22193023, L.W.C.), start-up fund from SUSTech (Y01216127 and Y01216227, Z.Z.), Distinguished Expert Fund From Nanshan District of Shenzhen (K19219502, Z.Z.), Shenzhen Municipal Science and Technology Innovation Committee (JCYJ20170817104736009, J.L.), Basic and Applied Basic Research Programs of Guangdong Province (2020A1515110990, L.Q.), China Postdoctoral Science Foundation (2018M640226, L.Q.), and SUSTech Presidential Postdoctoral Fellowship (L.Q.) is acknowledged. This work was also partly sponsored by Guangdong Provincial Key Laboratory of Catalysis (No. 2020B121201002), the Shenzhen Nobel Prize Scientists Laboratory Project (C17783101), Jilin Provincial Science Research Foundation of China (No. 20200403154SF), and the Center for Computational Science and Engineering, as well as the CHEM high performance supercomputer cluster (CHEM HPC) at the Southern University of Science and Technology. Publisher Copyright: {\textcopyright} 2022 American Chemical Society",
year = "2022",
month = feb,
day = "18",
doi = "10.1021/acscatal.1c05369",
language = "English (US)",
volume = "12",
pages = "2212--2222",
journal = "ACS Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "4",
}