Electrosynthesis of Atomically Precise Au Nanoclusters

Abstract Innovation in synthesis methodologies is crucial for advancing the discovery of new materials. This work reports the electrosynthesis of a [Au13(4‐tBuPhC≡C)2(Dppe)5]Cl3 nanocluster (Au13 NC) protected by alkynyl and phosphine ligands. From simple precursor, HAuCl4 and ligands, the whole syn...

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Main Authors: Jing Dong, Yawei Li, Yu Ding, Hai‐Feng Su, Xiaoqin Cui, Yu‐Xin Wang, Huan Li
Format: Article
Language:English
Published: Wiley 2025-05-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202414057
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author Jing Dong
Yawei Li
Yu Ding
Hai‐Feng Su
Xiaoqin Cui
Yu‐Xin Wang
Huan Li
author_facet Jing Dong
Yawei Li
Yu Ding
Hai‐Feng Su
Xiaoqin Cui
Yu‐Xin Wang
Huan Li
author_sort Jing Dong
collection DOAJ
description Abstract Innovation in synthesis methodologies is crucial for advancing the discovery of new materials. This work reports the electrosynthesis of a [Au13(4‐tBuPhC≡C)2(Dppe)5]Cl3 nanocluster (Au13 NC) protected by alkynyl and phosphine ligands. From simple precursor, HAuCl4 and ligands, the whole synthesis is driven by a constant potential in single electrolytic cell. X‐ray crystallography determines its total structure. Control experiments, cyclic voltammetry, Proton Nuclear Magnetic Resonance (1H NMR), gas chromatography, and other characterizations demonstrate that a critical tetranuclear Au(I) complex defines the electrochemical redox behavior of the reaction solution. The critical role of a base (e.g., triethylamine) is to suppress the hydrogen evolution reaction at the cathode, paving the way for the reduction of Au ions. To resolve the problem of over‐reduction and deposition of Au on the cathode, pulsed electrolysis, which is specific to electrosynthesis is employed. It significantly improves the reaction rate and the isolated yield of Au13. To extend the application scope, another four NCs protected by different ligands, [Au13(4‐FPhC≡C)2(Dppe)5]Cl3, [Au8(2‐CF3PhC≡C)2(Dppp)4](PF6)2, [Au11(Dppp)5]Cl3, and [Au8(SC2H4Ph)2(Dppp)4]Cl2 are synthesized electrochemically, demonstrating the versatility of the strategy.
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spelling doaj-art-735cb612770a49b3b88b7fe2df3640552025-08-20T03:48:47ZengWileyAdvanced Science2198-38442025-05-011217n/an/a10.1002/advs.202414057Electrosynthesis of Atomically Precise Au NanoclustersJing Dong0Yawei Li1Yu Ding2Hai‐Feng Su3Xiaoqin Cui4Yu‐Xin Wang5Huan Li6Institute of Crystalline Materials Shanxi University Taiyuan Shanxi 030006 ChinaSchool of Chemistry and Chemical Engineering Shanxi University Taiyuan Shanxi 030006 ChinaSchool of Chemistry and Chemical Engineering Shanxi University Taiyuan Shanxi 030006 ChinaDepartment of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. ChinaInstitute of Crystalline Materials Shanxi University Taiyuan Shanxi 030006 ChinaInstitute of Crystalline Materials Shanxi University Taiyuan Shanxi 030006 ChinaInstitute of Crystalline Materials Shanxi University Taiyuan Shanxi 030006 ChinaAbstract Innovation in synthesis methodologies is crucial for advancing the discovery of new materials. This work reports the electrosynthesis of a [Au13(4‐tBuPhC≡C)2(Dppe)5]Cl3 nanocluster (Au13 NC) protected by alkynyl and phosphine ligands. From simple precursor, HAuCl4 and ligands, the whole synthesis is driven by a constant potential in single electrolytic cell. X‐ray crystallography determines its total structure. Control experiments, cyclic voltammetry, Proton Nuclear Magnetic Resonance (1H NMR), gas chromatography, and other characterizations demonstrate that a critical tetranuclear Au(I) complex defines the electrochemical redox behavior of the reaction solution. The critical role of a base (e.g., triethylamine) is to suppress the hydrogen evolution reaction at the cathode, paving the way for the reduction of Au ions. To resolve the problem of over‐reduction and deposition of Au on the cathode, pulsed electrolysis, which is specific to electrosynthesis is employed. It significantly improves the reaction rate and the isolated yield of Au13. To extend the application scope, another four NCs protected by different ligands, [Au13(4‐FPhC≡C)2(Dppe)5]Cl3, [Au8(2‐CF3PhC≡C)2(Dppp)4](PF6)2, [Au11(Dppp)5]Cl3, and [Au8(SC2H4Ph)2(Dppp)4]Cl2 are synthesized electrochemically, demonstrating the versatility of the strategy.https://doi.org/10.1002/advs.202414057Au nanoclusterselectrosynthesispulsed electrolysis
spellingShingle Jing Dong
Yawei Li
Yu Ding
Hai‐Feng Su
Xiaoqin Cui
Yu‐Xin Wang
Huan Li
Electrosynthesis of Atomically Precise Au Nanoclusters
Advanced Science
Au nanoclusters
electrosynthesis
pulsed electrolysis
title Electrosynthesis of Atomically Precise Au Nanoclusters
title_full Electrosynthesis of Atomically Precise Au Nanoclusters
title_fullStr Electrosynthesis of Atomically Precise Au Nanoclusters
title_full_unstemmed Electrosynthesis of Atomically Precise Au Nanoclusters
title_short Electrosynthesis of Atomically Precise Au Nanoclusters
title_sort electrosynthesis of atomically precise au nanoclusters
topic Au nanoclusters
electrosynthesis
pulsed electrolysis
url https://doi.org/10.1002/advs.202414057
work_keys_str_mv AT jingdong electrosynthesisofatomicallypreciseaunanoclusters
AT yaweili electrosynthesisofatomicallypreciseaunanoclusters
AT yuding electrosynthesisofatomicallypreciseaunanoclusters
AT haifengsu electrosynthesisofatomicallypreciseaunanoclusters
AT xiaoqincui electrosynthesisofatomicallypreciseaunanoclusters
AT yuxinwang electrosynthesisofatomicallypreciseaunanoclusters
AT huanli electrosynthesisofatomicallypreciseaunanoclusters