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

Elliot J. Lawrence, Ewan R. Clark, Liam D. Curless, James M. Courtney, Robin J. Blagg, Michael J. Ingleson, Gregory G. Wildgoose

Research output: Contribution to journalArticlepeer-review

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.

Original languageEnglish
Pages (from-to)2537-2543
Number of pages7
JournalChemical Science
Volume7
Issue number4
DOIs
Publication statusE-pub ahead of print - 6 Jan 2016

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