期刊
CHEMICAL SCIENCE
卷 7, 期 4, 页码 2537-2543出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5sc04564a
关键词
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资金
- European Research Council under ERC Starting Grant [307061]
- ERC PoC Grant [640988]
- Leverhulme Trust
- Royal Society
- Engineering and Physical Sciences Research Council [1232343] Funding Source: researchfish
Whilst hydrogen is a potentially clean fuel for energy storage and utilisation technologies, its conversion to electricity comes at a high energetic cost. This demands the use of rare and expensive precious metal electrocatalysts. Electrochemical-frustrated Lewis pairs offer a metal-free, CO tolerant pathway to the electrocatalysis of hydrogen oxidation. They function by combining the hydrogen-activating ability of frustrated Lewis pairs (FLPs) with electrochemical oxidation of the resultant hydride. Here we present an electrochemical-FLP approach that utilises two different Lewis acids - a carbon-based N-methylacridinium cation that possesses excellent electrochemical attributes, and a borane that exhibits fast hydrogen cleavage kinetics and functions as a hydride shuttle. This synergistic interaction provides a system that is electrocatalytic with respect to the carbon-based Lewis acid, decreases the required potential for hydrogen oxidation by 1 V, and can be recycled multiple times.
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