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A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media / Gaia Neri, Iain Aldous, James J. Walsh, Laurence J. Hardwick, Alexander J. Cowan

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

Swansea University Author: Iain Aldous

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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
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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: College of Engineering
Issue: 2
Start Page: 1521
End Page: 1526