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Nano Research 2023, 16(3): 3641-3648 https://doi.org/10.1007/s12274-022-4288-4
Research Article | Issue | Published: 28 March 2022

Intramolecular hydroamination of alkynes driven by isomeric Au36(SR)24 nanocluster catalysts

Show Author's Information Yuying Zhang1,  Ancheng Tang1,  Xiao Cai1,  Jiayu Xu1,  Guangjun Li1,  Weigang Hu1,  Xu Liu1,  Mingyang Chen2( ),  Yan Zhu1( )
School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
Center for Green Innovation, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China
Keywords:
catalytic activity, catalysis, isomeric structure, Au36 clusters
Topics:
Nanocatalysts
Cite this article:
Zhang Y, Tang A, Cai X, et al. Intramolecular hydroamination of alkynes driven by isomeric Au36(SR)24 nanocluster catalysts. Nano Research, 2023, 16(3): 3641-3648. https://doi.org/10.1007/s12274-022-4288-4
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Abstract Full text Electronic supplementary material About this article

It remains elusive to realize the distinct catalysis of isomeric catalysts because it becomes challenging to identify structural isomers in the polydisperse nanoparticles. Herein we investigate catalysis of two geometric isomers for 36-gold-atom nanoclusters with different Au cores arrangements but the same thiolate ligands, thereby providing access to isomer catalysts readily participate in a desired reaction. Compared to the Au36(SR)24 with a one-dimensional (1D) layout of Au4 tetrahedral units, the Au36(SR)24 with a two-dimensional (2D) layout of Au4 tetrahedral units is more effective for the intramolecular hydroamination of alkyne. Our study suggests that the exposed Au sties of the two Au36(SR)24 catalysts favor different reaction intermediates and pathways. The intramolecular H transfer leads to intermediates with the C–N and with C=N for the 1D and 2D Au36(SR)24 respectively, and hence the different on-site and off-site pathways for the successive reaction steps account for the different performances of the two Au36(SR)24 catalysts.


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About this article

Intramolecular hydroamination of alkynes driven by isomeric Au36(SR)24 nanocluster catalysts

Show Author's information Yuying Zhang1, Ancheng Tang1, Xiao Cai1, Jiayu Xu1, Guangjun Li1, Weigang Hu1, Xu Liu1, Mingyang Chen2( ), Yan Zhu1( )
School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
Center for Green Innovation, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China

Abstract

It remains elusive to realize the distinct catalysis of isomeric catalysts because it becomes challenging to identify structural isomers in the polydisperse nanoparticles. Herein we investigate catalysis of two geometric isomers for 36-gold-atom nanoclusters with different Au cores arrangements but the same thiolate ligands, thereby providing access to isomer catalysts readily participate in a desired reaction. Compared to the Au36(SR)24 with a one-dimensional (1D) layout of Au4 tetrahedral units, the Au36(SR)24 with a two-dimensional (2D) layout of Au4 tetrahedral units is more effective for the intramolecular hydroamination of alkyne. Our study suggests that the exposed Au sties of the two Au36(SR)24 catalysts favor different reaction intermediates and pathways. The intramolecular H transfer leads to intermediates with the C–N and with C=N for the 1D and 2D Au36(SR)24 respectively, and hence the different on-site and off-site pathways for the successive reaction steps account for the different performances of the two Au36(SR)24 catalysts.

Keywords: catalytic activity, catalysis, isomeric structure, Au36 clusters

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Acknowledgements

Publication history

Received: 17 December 2021
Revised: 01 March 2022
Accepted: 03 March 2022
Published: 28 March 2022
Issue date: March 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We acknowledge financial supports from Fundamental Research Funds for the Central Universities, Programs for high-level entrepreneurial and innovative talents introduction of Jiangsu Province, and Scientific and Technological Innovation Foundation of Shunde Graduate School of USTB (No. BK19BE024). This computational work is supported by the Tianhe2-JK computing time award at the Beijing Computational Science Research Center.

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