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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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first_indexed 2019-08-09T16:32:05Z
last_indexed 2019-08-09T16:32:05Z
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spelling 2019-08-07T12:30:34.8850811 v2 51336 2019-08-06 A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media 87867d675f1cd66804b1c6c2626cac24 Iain Aldous Iain Aldous true false 2019-08-06 CHEG 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. Journal Article Chemical Science 7 2 1521 1526 2041-6520 2041-6539 31 12 2016 2016-12-31 10.1039/C5SC03225C COLLEGE NANME Chemical Engineering COLLEGE CODE CHEG Swansea University 2019-08-07T12:30:34.8850811 2019-08-06T21:14:42.6387422 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Gaia Neri 1 Iain Aldous 2 James J. Walsh 3 Laurence J. Hardwick 4 Alexander J. Cowan 5
title A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
spellingShingle A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
Iain Aldous
title_short A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
title_full A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
title_fullStr A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
title_full_unstemmed A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
title_sort A highly active nickel electrocatalyst shows excellent selectivity for CO2 reduction in acidic media
author_id_str_mv 87867d675f1cd66804b1c6c2626cac24
author_id_fullname_str_mv 87867d675f1cd66804b1c6c2626cac24_***_Iain Aldous
author Iain Aldous
author2 Gaia Neri
Iain Aldous
James J. Walsh
Laurence J. Hardwick
Alexander J. Cowan
format Journal article
container_title Chemical Science
container_volume 7
container_issue 2
container_start_page 1521
publishDate 2016
institution Swansea University
issn 2041-6520
2041-6539
doi_str_mv 10.1039/C5SC03225C
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str 0
active_str 0
description 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.
published_date 2016-12-31T04:03:11Z
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score 11.036706

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