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Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction
Colloidally synthesised nanocrystals (NCs) are increasingly utilised as catalysts to drive both thermal and electrocatalytic reactions. Their well-defined size and shape, controlled by organic ligands, are ideal to identify the parameters relevant to the activity, selectivity and stability in cataly...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8161676/ https://www.ncbi.nlm.nih.gov/pubmed/34094200 http://dx.doi.org/10.1039/d0sc03061a |
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author | Pankhurst, James R. Iyengar, Pranit Loiudice, Anna Mensi, Mounir Buonsanti, Raffaella |
author_facet | Pankhurst, James R. Iyengar, Pranit Loiudice, Anna Mensi, Mounir Buonsanti, Raffaella |
author_sort | Pankhurst, James R. |
collection | PubMed |
description | Colloidally synthesised nanocrystals (NCs) are increasingly utilised as catalysts to drive both thermal and electrocatalytic reactions. Their well-defined size and shape, controlled by organic ligands, are ideal to identify the parameters relevant to the activity, selectivity and stability in catalysis. However, the impact of the native surface ligands during catalysis still remains poorly understood, as does their fate. CuNCs are among the state-of-the-art catalysts for the electrochemical CO(2) reduction reaction (CO(2)RR). In this work, we study CuNCs that are capped by different organic ligands to investigate their impact on the catalytic properties. We show that the latter desorb from the surface at a cathodic potential that depends on their binding strength with the metal surface, rather than their own electroreduction potentials. By monitoring the evolving surface chemistry in situ, we find that weakly bound ligands desorb very rapidly while strongly bound ligands impact the catalytic performance. This work provides a criterion to select labile ligands versus ligands that will persist on the surface, thus offering opportunity for interface design. |
format | Online Article Text |
id | pubmed-8161676 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-81616762021-06-04 Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction Pankhurst, James R. Iyengar, Pranit Loiudice, Anna Mensi, Mounir Buonsanti, Raffaella Chem Sci Chemistry Colloidally synthesised nanocrystals (NCs) are increasingly utilised as catalysts to drive both thermal and electrocatalytic reactions. Their well-defined size and shape, controlled by organic ligands, are ideal to identify the parameters relevant to the activity, selectivity and stability in catalysis. However, the impact of the native surface ligands during catalysis still remains poorly understood, as does their fate. CuNCs are among the state-of-the-art catalysts for the electrochemical CO(2) reduction reaction (CO(2)RR). In this work, we study CuNCs that are capped by different organic ligands to investigate their impact on the catalytic properties. We show that the latter desorb from the surface at a cathodic potential that depends on their binding strength with the metal surface, rather than their own electroreduction potentials. By monitoring the evolving surface chemistry in situ, we find that weakly bound ligands desorb very rapidly while strongly bound ligands impact the catalytic performance. This work provides a criterion to select labile ligands versus ligands that will persist on the surface, thus offering opportunity for interface design. The Royal Society of Chemistry 2020-08-17 /pmc/articles/PMC8161676/ /pubmed/34094200 http://dx.doi.org/10.1039/d0sc03061a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Pankhurst, James R. Iyengar, Pranit Loiudice, Anna Mensi, Mounir Buonsanti, Raffaella Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title | Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title_full | Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title_fullStr | Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title_full_unstemmed | Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title_short | Metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical CO(2) reduction reaction |
title_sort | metal–ligand bond strength determines the fate of organic ligands on the catalyst surface during the electrochemical co(2) reduction reaction |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8161676/ https://www.ncbi.nlm.nih.gov/pubmed/34094200 http://dx.doi.org/10.1039/d0sc03061a |
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