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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
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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 0000-0003-4776-9573 Iain Aldous Iain Aldous true false 2019-08-06 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 COLLEGE CODE 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 0000-0003-4776-9573 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 2016-12-31T13:53:21Z
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score 11.048129

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