Cargando…

Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu

Intensive research in electrochemical CO(2) reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products sel...

Descripción completa

Detalles Bibliográficos
Autores principales: Lim, Carina Yi Jing, Yilmaz, Meltem, Arce-Ramos, Juan Manuel, Handoko, Albertus D., Teh, Wei Jie, Zheng, Yuangang, Khoo, Zi Hui Jonathan, Lin, Ming, Isaacs, Mark, Tam, Teck Lip Dexter, Bai, Yang, Ng, Chee Koon, Yeo, Boon Siang, Sankar, Gopinathan, Parkin, Ivan P., Hippalgaonkar, Kedar, Sullivan, Michael B., Zhang, Jia, Lim, Yee-Fun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9860078/
https://www.ncbi.nlm.nih.gov/pubmed/36670095
http://dx.doi.org/10.1038/s41467-023-35912-7
_version_ 1784874494890868736
author Lim, Carina Yi Jing
Yilmaz, Meltem
Arce-Ramos, Juan Manuel
Handoko, Albertus D.
Teh, Wei Jie
Zheng, Yuangang
Khoo, Zi Hui Jonathan
Lin, Ming
Isaacs, Mark
Tam, Teck Lip Dexter
Bai, Yang
Ng, Chee Koon
Yeo, Boon Siang
Sankar, Gopinathan
Parkin, Ivan P.
Hippalgaonkar, Kedar
Sullivan, Michael B.
Zhang, Jia
Lim, Yee-Fun
author_facet Lim, Carina Yi Jing
Yilmaz, Meltem
Arce-Ramos, Juan Manuel
Handoko, Albertus D.
Teh, Wei Jie
Zheng, Yuangang
Khoo, Zi Hui Jonathan
Lin, Ming
Isaacs, Mark
Tam, Teck Lip Dexter
Bai, Yang
Ng, Chee Koon
Yeo, Boon Siang
Sankar, Gopinathan
Parkin, Ivan P.
Hippalgaonkar, Kedar
Sullivan, Michael B.
Zhang, Jia
Lim, Yee-Fun
author_sort Lim, Carina Yi Jing
collection PubMed
description Intensive research in electrochemical CO(2) reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO(2) reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO(2) reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids.
format Online
Article
Text
id pubmed-9860078
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-98600782023-01-22 Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu Lim, Carina Yi Jing Yilmaz, Meltem Arce-Ramos, Juan Manuel Handoko, Albertus D. Teh, Wei Jie Zheng, Yuangang Khoo, Zi Hui Jonathan Lin, Ming Isaacs, Mark Tam, Teck Lip Dexter Bai, Yang Ng, Chee Koon Yeo, Boon Siang Sankar, Gopinathan Parkin, Ivan P. Hippalgaonkar, Kedar Sullivan, Michael B. Zhang, Jia Lim, Yee-Fun Nat Commun Article Intensive research in electrochemical CO(2) reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO(2) reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO(2) reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids. Nature Publishing Group UK 2023-01-20 /pmc/articles/PMC9860078/ /pubmed/36670095 http://dx.doi.org/10.1038/s41467-023-35912-7 Text en © The Author(s) 2023, corrected publication 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Lim, Carina Yi Jing
Yilmaz, Meltem
Arce-Ramos, Juan Manuel
Handoko, Albertus D.
Teh, Wei Jie
Zheng, Yuangang
Khoo, Zi Hui Jonathan
Lin, Ming
Isaacs, Mark
Tam, Teck Lip Dexter
Bai, Yang
Ng, Chee Koon
Yeo, Boon Siang
Sankar, Gopinathan
Parkin, Ivan P.
Hippalgaonkar, Kedar
Sullivan, Michael B.
Zhang, Jia
Lim, Yee-Fun
Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title_full Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title_fullStr Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title_full_unstemmed Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title_short Surface charge as activity descriptors for electrochemical CO(2) reduction to multi-carbon products on organic-functionalised Cu
title_sort surface charge as activity descriptors for electrochemical co(2) reduction to multi-carbon products on organic-functionalised cu
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9860078/
https://www.ncbi.nlm.nih.gov/pubmed/36670095
http://dx.doi.org/10.1038/s41467-023-35912-7
work_keys_str_mv AT limcarinayijing surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT yilmazmeltem surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT arceramosjuanmanuel surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT handokoalbertusd surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT tehweijie surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT zhengyuangang surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT khoozihuijonathan surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT linming surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT isaacsmark surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT tamtecklipdexter surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT baiyang surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT ngcheekoon surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT yeoboonsiang surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT sankargopinathan surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT parkinivanp surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT hippalgaonkarkedar surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT sullivanmichaelb surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT zhangjia surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu
AT limyeefun surfacechargeasactivitydescriptorsforelectrochemicalco2reductiontomulticarbonproductsonorganicfunctionalisedcu