期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 5, 期 7, 页码 7737-7740出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2ee21123h
关键词
-
资金
- MIT Energy Initiative for a predoctoral fellowship
- DOE [DE-FG02-05ER15745]
Cobalt hangman porphyrins catalyze the hydrogen evolution reaction (HER). The hangman group is observed to facilitate HER by mediating a proton-coupled electron transfer (PCET) reaction. The details of the PCET pathway have been determined by comparing rate constants associated with the ET and PT processes of the hangman system to those of the corresponding values measured for porphyrins that lack an internal proton relay. A rapid intramolecular proton transfer from the carboxylic acid hanging group to the reduced cobalt centre of 8.5 x 10(6) s(-1) provides a facile pathway for the formation of Co(II) H, which leads directly to H-2 generation.
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