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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...

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Autores principales: Pankhurst, James R., Iyengar, Pranit, Loiudice, Anna, Mensi, Mounir, Buonsanti, Raffaella
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2020
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.
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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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