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

Lawrence, Elliot J., Clark, Ewan R., Curless, Liam D., Courtney, James M., Blagg, Robin J., Ingleson, Michael J., Wildgoose, Gregory G. (2016) Metal-free electrocatalytic hydrogen oxidation using frustrated Lewis pairs and carbon-based Lewis acids. Chemical Science, 7 (4). pp. 2537-2543. ISSN 2041-6520. (doi:10.1039/C5SC04564A)

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http://dx.doi.org/10.1039/C5SC04564A

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.

Item Type: Article
DOI/Identification number: 10.1039/C5SC04564A
Divisions: Faculties > Sciences > School of Physical Sciences
Depositing User: Ewan Clark
Date Deposited: 23 Jan 2017 16:34 UTC
Last Modified: 29 May 2019 18:35 UTC
Resource URI: https://kar.kent.ac.uk/id/eprint/60045 (The current URI for this page, for reference purposes)
Clark, Ewan R.: https://orcid.org/0000-0001-7287-2631
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