期刊
ACS CATALYSIS
卷 8, 期 4, 页码 3286-3296出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b04379
关键词
electrocatalysis; hydrogen; scaling relation; overpotential; nickel; proton relay; viscosity
资金
- Center for Molecular Electrocatalysis, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences
A longstanding challenge in molecular electrocatalysis is to design catalysts that break away from the tradeoff between rate and overpotential arising from electronic scaling relationships. Here we report an inversion of the rate-over-potential correlation through system-level design of [Ni-((P2N2R')-N-R)(2)](2+) electrocatalysts for the production of H-2. The overpotential is lowered by an electron-withdrawing ligand, while the turnover frequency is increased by controlling the catalyst structural dynamics, using both ligand design and solvent viscosity. The cumulative effect of controlling each of these system components is an electrocatalyst with a turnover frequency of 70000 s(-1) and an overpotential of 230 mV, corresponding to a 100-fold rate enhancement and a 170 mV reduction in overpotential in comparison to the parent nickel catalyst. Molecular Tafel plot analysis reveals that the new catalysts reported here are substantially more efficient than other leading molecular electrocatalysts for the production of H-2.
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