Issue 2, 2016

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

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.

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

Supplementary files

Article information

Article type
Edge Article
Submitted
01 Sep 2015
Accepted
20 Nov 2015
First published
24 Nov 2015
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2016,7, 1521-1526

Author version available

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

G. Neri, I. M. Aldous, J. J. Walsh, L. J. Hardwick and A. J. Cowan, Chem. Sci., 2016, 7, 1521 DOI: 10.1039/C5SC03225C

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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