期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 3, 页码 1109-1115出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja509779q
关键词
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资金
- Center for Bio-Inspired Solar Fuel Production, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001016]
- National Science Foundation of the XAS [CHE-1362662]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- Case Center for Synchrotron Biosciences
- National Institute of Biomedical Imaging and Bioengineering (NIH) [P30-EB-009998]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1362662] Funding Source: National Science Foundation
Here we report the electrocatalytic reduction of protons to hydrogen by a novel S2P2 coordinated nickel complex, [Ni(bdt)(dppf)] (bdt = 1,2-benzenedithiolate, dppf = 1,1'-bis(diphenylphosphino)ferrocene). The catalysis is fast and efficient with a turnover frequency of 1240 s(-1) and an overpotential of only 265 mV for half activity at low acid concentrations. Furthermore, catalysis is possible using a weak acid, and the complex is stable for at least 4 h in acidic solution. Calculations of the system carried out at the density functional level of theory (DFT) are consistent with a mechanism for catalysis in which both protonations take place at the nickel center.
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