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. and 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

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Abstract

Whilst hydrogen is a potentially clean fuel for energy storage and utilization 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 utilizes 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
Additional Information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Faculty \ School: Faculty of Science > School of Chemistry
Depositing User: Pure Connector
Date Deposited: 18 Feb 2016 15:00
Last Modified: 04 Nov 2020 00:42
URI: https://ueaeprints.uea.ac.uk/id/eprint/57184
DOI: 10.1039/C5SC04564A

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