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具有优异电催化析氢反应活性的原子精确AuPt(硫醇盐)(二硫醇盐)纳米团簇

Atomically Precise AuPt(thiolate)(dithiolate) Nanoclusters with Excellent Electrocatalytic Hydrogen Evolution Reactivity.

作者信息

Sera Miyu, Hossain Sakiat, Yoshikawa Sara, Takemae Kana, Ikeda Ayaka, Tanaka Tomoya, Kosaka Taiga, Niihori Yoshiki, Kawawaki Tokuhisa, Negishi Yuichi

机构信息

Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, Kagurazaka, Shinjuku-ku, Tokyo 162-8601, Japan.

Research Institute for Science & Technology, Tokyo University of Science, Kagurazaka, Shinjuku-ku, Tokyo 162-8601, Japan.

出版信息

J Am Chem Soc. 2024 Oct 30;146(43):29684-29693. doi: 10.1021/jacs.4c10868. Epub 2024 Oct 15.

DOI:10.1021/jacs.4c10868
PMID:39405364
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11613320/
Abstract

[AuPt(C6)] (C6 = 1-hexanethiolate) is twice as active as commercial Pt nanoparticles in promoting the electrocatalytic hydrogen evolution reaction (HER), thereby attracting attention as new HER catalysts with well-controlled geometric structures. In this study, we succeeded in synthesizing two new Au-Pt alloy nanoclusters, namely, [AuPt(TBBT)(TDT)] (TBBT = 4--butylbenzenethiolate; TDT = thiodithiolate) and [AuPt(TBBT)(PDT)] (PDT = 1,3-propanedithiolate), by exchanging all the ligands of [AuPt(PET)] (PET = 2-phenylethanethiolate) with mono- or dithiolates. Although [AuPt(TBBT)(TDT)] was synthesized serendipitously, a similar cluster, [AuPt(TBBT)(PDT)], was subsequently obtained by selecting the appropriate reaction conditions and optimal combination of thiolate and dithiolate ligands. Single crystal X-ray diffraction analyses revealed that the lengths and orientations of -Au(I)-SR-Au(I)- staples in [AuPt(TBBT)(TDT)] and [AuPt(TBBT)(PDT)] were different from those in [AuPt(C6)], [AuPt(PET)], and [AuPt(TBBT)], and these subtle differences were reflected in the geometric and electronic structures as well as the HER activities of [AuPt(TBBT)(TDT)] and [AuPt(TBBT)(PDT)]. Accordingly, the HER activities of products [AuPt(TBBT)(TDT)] and [AuPt(TBBT)(PDT)] were, respectively, 3.5 and 4.9 times higher than those of [AuPt(C6)] and [AuPt(TBBT)].

摘要

[AuPt(C6)]（C6 = 己硫醇盐）在促进电催化析氢反应（HER）方面的活性是商业铂纳米颗粒的两倍，因此作为具有良好控制几何结构的新型HER催化剂受到关注。在本研究中，我们通过用单硫醇盐或二硫醇盐交换[AuPt(PET)]（PET = 苯乙硫醇盐）的所有配体，成功合成了两种新的金 - 铂合金纳米团簇，即[AuPt(TBBT)(TDT)]（TBBT = 对叔丁基苯硫醇盐；TDT = 硫代二硫醇盐）和[AuPt(TBBT)(PDT)]（PDT = 1,3 - 丙二硫醇盐）。虽然[AuPt(TBBT)(TDT)]是偶然合成的，但随后通过选择合适的反应条件以及硫醇盐和二硫醇盐配体的最佳组合获得了类似的团簇[AuPt(TBBT)(PDT)]。单晶X射线衍射分析表明，[AuPt(TBBT)(TDT)]和[AuPt(TBBT)(PDT)]中 -Au(I)-SR-Au(I)- 主链的长度和取向与[AuPt(C6)]、[AuPt(PET)]和[AuPt(TBBT)]中的不同，这些细微差异反映在[AuPt(TBBT)(TDT)]和[AuPt(TBBT)(PDT)]的几何和电子结构以及HER活性中。因此，产物[AuPt(TBBT)(TDT)]和[AuPt(TBBT)(PDT)]的HER活性分别比[AuPt(C6)]和[AuPt(TBBT)]高3.5倍和4.9倍。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/43922f7a935b/ja4c10868_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/578159ce542b/ja4c10868_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/733a5a6e1a1b/ja4c10868_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/70f868e4ef14/ja4c10868_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/3ea8a12f025f/ja4c10868_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/933b6ccc26cb/ja4c10868_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/8c5b5002860b/ja4c10868_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/43922f7a935b/ja4c10868_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/578159ce542b/ja4c10868_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/733a5a6e1a1b/ja4c10868_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/70f868e4ef14/ja4c10868_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/3ea8a12f025f/ja4c10868_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/933b6ccc26cb/ja4c10868_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/8c5b5002860b/ja4c10868_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f251/11613320/43922f7a935b/ja4c10868_0006.jpg

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本文引用的文献

[1]
Combined experimental and computational study of the photoabsorption of the monodoped and nondoped nanoclusters AuPt(SR), AgPt(SR), and Ag(SR).

Phys Chem Chem Phys. 2024-6-26

[2]
Chemical Flexibility of Atomically Precise Metal Clusters.

Chem Rev. 2024-6-12

[3]
Regulating the Electronic Structure of Metal Nanoclusters by Longitudinal Single-Dithiolate Substitution.

J Phys Chem Lett. 2023-4-6

[4]
Mechanism of Cations Suppressing Proton Diffusion Kinetics for Electrocatalysis.

Angew Chem Int Ed Engl. 2023-3-27

[5]
Selective formation of [Au(SPh Bu)], [AuPd(SPh Bu)] and [AuPt(SCHPh)(SPh Bu)] by controlling ligand-exchange reaction.

Chem Sci. 2022-3-30

[6]
Resolving the Structural Debate for the Hydrated Excess Proton in Water.

J Am Chem Soc. 2021-11-10

[7]
Self-promoted solid-state covalent networking of Au(SR) through reversible disulfide bonds. A critical effect of the nanocluster in oxidation processes.

Nanoscale. 2021-6-14

[8]
Cluster From Cluster: A Quantitative Approach to Magic Gold Nanoclusters [Au (SR) ].

Angew Chem Int Ed Engl. 2021-6-21

[9]
Toward Active-Site Tailoring in Heterogeneous Catalysis by Atomically Precise Metal Nanoclusters with Crystallographic Structures.

Chem Rev. 2021-1-27

[10]
Gold nanoclusters as electrocatalysts: size, ligands, heteroatom doping, and charge dependences.

Nanoscale. 2020-5-14

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