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A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media

Gaia Neri, Iain Aldous Orcid Logo, James J. Walsh, Laurence J. Hardwick, Alexander J. Cowan

Chemical Science, Volume: 7, Issue: 2, Pages: 1521 - 1526

Swansea University Author: Iain Aldous Orcid Logo

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DOI (Published version): 10.1039/C5SC03225C

Abstract

The development of selective electrocatalysts for CO2 reduction in water offers a sustainable route to carbon based fuels and feedstocks. However, molecular catalysts are typically studied in non-aqueous solvents, in part to avoid competitive H2 evolution. [Ni(cyclam)]2+ (1) is one of the few known...

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Published in: Chemical Science
ISSN: 2041-6520 2041-6539
Published: 2016
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URI: https://cronfa.swan.ac.uk/Record/cronfa51336
Abstract: The development of selective electrocatalysts for CO2 reduction in water offers a sustainable route to carbon based fuels and feedstocks. However, molecular catalysts are typically studied in non-aqueous solvents, in part to avoid competitive H2 evolution. [Ni(cyclam)]2+ (1) is one of the few known electrocatalysts that operate in water and 30 years after its report its activity remains a rarely surpassed benchmark. Here we report that [Ni(cyclam-CO2H)]2+ (cyclam-CO2H = 1,4,8,11-tetraazacyclotetradecane-6-carboxylic acid (2)) shows greatly enhanced activity versus1 for CO production. At pHs < pKa of the pendant carboxylic acid a large increase in catalytic activity occurs. Remarkably, despite the high proton concentration (pH 2), 2 maintains selectivity for CO2 reduction and is believed to be unique in operating selectively in such acidic aqueous solutions.
College: Faculty of Science and Engineering
Issue: 2
Start Page: 1521
End Page: 1526