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Issue 4, 2016
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Metal-free electrocatalytic hydrogen oxidation using frustrated Lewis pairs and carbon-based Lewis acids

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Abstract

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.

Graphical abstract: Metal-free electrocatalytic hydrogen oxidation using frustrated Lewis pairs and carbon-based Lewis acids

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Publication details

The article was received on 27 Nov 2015, accepted on 06 Jan 2016 and first published on 06 Jan 2016


Article type: Edge Article
DOI: 10.1039/C5SC04564A
Citation: Chem. Sci., 2016,7, 2537-2543
  • Open access: Creative Commons BY license
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    Metal-free electrocatalytic hydrogen oxidation using frustrated Lewis pairs and carbon-based Lewis acids

    E. J. Lawrence, E. R. Clark, L. D. Curless, J. M. Courtney, R. J. Blagg, M. J. Ingleson and G. G. Wildgoose, Chem. Sci., 2016, 7, 2537
    DOI: 10.1039/C5SC04564A

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