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Control of single-ligand chemistry on thiolated Au(25) nanoclusters

Diverse methods have been developed to tailor the number of metal atoms in metal nanoclusters, but control of surface ligand number at a given cluster size is rare. Here we demonstrate that reversible addition and elimination of a single surface thiolate ligand (-SR) on gold nanoclusters can be real...

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Autores principales: Cao, Yitao, Fung, Victor, Yao, Qiaofeng, Chen, Tiankai, Zang, Shuangquan, Jiang, De-en, Xie, Jianping
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7603303/
https://www.ncbi.nlm.nih.gov/pubmed/33127904
http://dx.doi.org/10.1038/s41467-020-19327-2
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author Cao, Yitao
Fung, Victor
Yao, Qiaofeng
Chen, Tiankai
Zang, Shuangquan
Jiang, De-en
Xie, Jianping
author_facet Cao, Yitao
Fung, Victor
Yao, Qiaofeng
Chen, Tiankai
Zang, Shuangquan
Jiang, De-en
Xie, Jianping
author_sort Cao, Yitao
collection PubMed
description Diverse methods have been developed to tailor the number of metal atoms in metal nanoclusters, but control of surface ligand number at a given cluster size is rare. Here we demonstrate that reversible addition and elimination of a single surface thiolate ligand (-SR) on gold nanoclusters can be realized, opening the door to precision ligand engineering on atomically precise nanoclusters. We find that oxidative etching of [Au(25)SR(18)](−) nanoclusters adds an excess thiolate ligand and generates a new species, [Au(25)SR(19)](0). The addition reaction can be reversed by CO reduction of [Au(25)SR(19)](0), leading back to [Au(25)SR(18)](−) and eliminating precisely one surface ligand. Intriguingly, we show that the ligand shell of Au(25) nanoclusters becomes more fragile and rigid after ligand addition. This reversible addition/elimination reaction of a single surface ligand on gold nanoclusters shows potential to precisely control the number of surface ligands and to explore new ligand space at each nuclearity.
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spelling pubmed-76033032020-11-10 Control of single-ligand chemistry on thiolated Au(25) nanoclusters Cao, Yitao Fung, Victor Yao, Qiaofeng Chen, Tiankai Zang, Shuangquan Jiang, De-en Xie, Jianping Nat Commun Article Diverse methods have been developed to tailor the number of metal atoms in metal nanoclusters, but control of surface ligand number at a given cluster size is rare. Here we demonstrate that reversible addition and elimination of a single surface thiolate ligand (-SR) on gold nanoclusters can be realized, opening the door to precision ligand engineering on atomically precise nanoclusters. We find that oxidative etching of [Au(25)SR(18)](−) nanoclusters adds an excess thiolate ligand and generates a new species, [Au(25)SR(19)](0). The addition reaction can be reversed by CO reduction of [Au(25)SR(19)](0), leading back to [Au(25)SR(18)](−) and eliminating precisely one surface ligand. Intriguingly, we show that the ligand shell of Au(25) nanoclusters becomes more fragile and rigid after ligand addition. This reversible addition/elimination reaction of a single surface ligand on gold nanoclusters shows potential to precisely control the number of surface ligands and to explore new ligand space at each nuclearity. Nature Publishing Group UK 2020-10-30 /pmc/articles/PMC7603303/ /pubmed/33127904 http://dx.doi.org/10.1038/s41467-020-19327-2 Text en © The Author(s) 2020 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/.
spellingShingle Article
Cao, Yitao
Fung, Victor
Yao, Qiaofeng
Chen, Tiankai
Zang, Shuangquan
Jiang, De-en
Xie, Jianping
Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title_full Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title_fullStr Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title_full_unstemmed Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title_short Control of single-ligand chemistry on thiolated Au(25) nanoclusters
title_sort control of single-ligand chemistry on thiolated au(25) nanoclusters
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7603303/
https://www.ncbi.nlm.nih.gov/pubmed/33127904
http://dx.doi.org/10.1038/s41467-020-19327-2
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