Metal-free dihydrogen oxidation by a borenium cation: A combined electrochemical/frustrated Lewis pair approach

Lawrence, Elliot J., Herrington, Thomas J., Ashley, Andrew E. and Wildgoose, Gregory G. (2014) Metal-free dihydrogen oxidation by a borenium cation: A combined electrochemical/frustrated Lewis pair approach. Angewandte Chemie-International Edition, 53 (37). 9922–9925. ISSN 1433-7851

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Abstract

In order to use H2 as a clean source of electricity, prohibitively rare and expensive precious metal electrocatalysts, such as Pt, are often used to overcome the large oxidative voltage required to convert H2 into 2 H+ and 2 e−. Herein, we report a metal-free approach to catalyze the oxidation of H2 by combining the ability of frustrated Lewis pairs (FLPs) to heterolytically cleave H2 with the in situ electrochemical oxidation of the resulting borohydride. The use of the NHC-stabilized borenium cation [(IiPr2)(BC8H14)]+ (IiPr2=C3H2(NiPr)2, NHC=N-heterocyclic carbene) as the Lewis acidic component of the FLP is shown to decrease the voltage required for H2 oxidation by 910 mV at inexpensive carbon electrodes, a significant energy saving equivalent to 175.6 kJ mol−1. The NHC–borenium Lewis acid also offers improved catalyst recyclability and chemical stability compared to B(C6F5)3, the paradigm Lewis acid originally used to pioneer our combined electrochemical/frustrated Lewis pair approach.

Item Type:	Article
Additional Information:	© 2014 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited
Uncontrolled Keywords:	borenium cations,electrocatalysis,frustrated lewis pairs,hydrogen,oxidation
Faculty \ School:	Faculty of Science Faculty of Science > School of Chemistry
UEA Research Groups:	Faculty of Science > Research Groups > Physical and Analytical Chemistry (former - to 2017) Faculty of Science > Research Groups > Synthetic Chemistry (former - to 2017)
Depositing User:	Pure Connector
Date Deposited:	25 Jul 2014 14:54
Last Modified:	29 Mar 2024 00:49
URI:	https://ueaeprints.uea.ac.uk/id/eprint/49748
DOI:	10.1002/anie.201405721

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