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Nano Research 2023, 16(5): 6507-6511 https://doi.org/10.1007/s12274-022-5279-1
Communication | Issue | Published: 27 December 2022

In-situ reconstruction of single-atom Pt on Co3O4 for hydrogenation

Show Author's Information Sai Zhang1,2( ),  Zhaoming Xia3( ),  Wenbin Li1,  You Wang1,  Yong Zou1,  Mingkai Zhang1,  Zhongmiao Gong4,  Yi Cui4,  Yongquan Qu1( )
Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an 710072, China
Research & Development Institute of Northwestern Polytechnical University in Shenzhen, Shenzhen 518057, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China
Keywords:
coordination environment, hydrogenation, single-atom catalysis (SACs), Pt-Co bimetallic sites
Topics:
Catalytic
Cite this article:
Zhang S, Xia Z, Li W, et al. In-situ reconstruction of single-atom Pt on Co3O4 for hydrogenation. Nano Research, 2023, 16(5): 6507-6511. https://doi.org/10.1007/s12274-022-5279-1
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Abstract Full text Electronic supplementary material About this article

Actual chemical states of single-atom metal on reducible supports remain a fiercely debated topic under reactive environments. Herein, we demonstrate that the single-atom Pt on Co3O4 surface undergoes an in-situ reconstruction to form isolated Pt-Co bimetallic sites via reducing coordination number of Pt–O in the presence of hydrogen from both simulations and in-situ X-ray photoelectron spectroscopy. The modified chemical states of Pt greatly promoted H2 activation, thus delivering a significantly high turnover frequency of 7,448 h−1 (19.5 times over Pt nanoparticles on Co3O4) for hydrogenation of cinnamaldehyde. The satisfactory selectivity of 95.2% towards cinnamyl alcohol was ascribed to a tilted adsorption configuration of reactant on the catalyst surface via aldehyde group. We anticipate that the recognitions on in-situ reconstruction of single-atom catalysts (SACs) under the reducing conditions benefit the design of highly-performed hydrogenation catalysts.


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Electronic supplementary material
About this article

In-situ reconstruction of single-atom Pt on Co3O4 for hydrogenation

Show Author's information Sai Zhang1,2( ), Zhaoming Xia3( ), Wenbin Li1, You Wang1, Yong Zou1, Mingkai Zhang1, Zhongmiao Gong4, Yi Cui4, Yongquan Qu1( )
Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an 710072, China
Research & Development Institute of Northwestern Polytechnical University in Shenzhen, Shenzhen 518057, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China

Abstract

Actual chemical states of single-atom metal on reducible supports remain a fiercely debated topic under reactive environments. Herein, we demonstrate that the single-atom Pt on Co3O4 surface undergoes an in-situ reconstruction to form isolated Pt-Co bimetallic sites via reducing coordination number of Pt–O in the presence of hydrogen from both simulations and in-situ X-ray photoelectron spectroscopy. The modified chemical states of Pt greatly promoted H2 activation, thus delivering a significantly high turnover frequency of 7,448 h−1 (19.5 times over Pt nanoparticles on Co3O4) for hydrogenation of cinnamaldehyde. The satisfactory selectivity of 95.2% towards cinnamyl alcohol was ascribed to a tilted adsorption configuration of reactant on the catalyst surface via aldehyde group. We anticipate that the recognitions on in-situ reconstruction of single-atom catalysts (SACs) under the reducing conditions benefit the design of highly-performed hydrogenation catalysts.

Keywords: coordination environment, hydrogenation, single-atom catalysis (SACs), Pt-Co bimetallic sites

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Publication history
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Acknowledgements

Publication history

Received: 30 July 2022
Revised: 01 November 2022
Accepted: 01 November 2022
Published: 27 December 2022
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We acknowledge the National Natural Science Foundation of China (Nos. 21872109 and 22002115). S. Z. is also supported by the Guangdong Basic and Applied Basic Research Foundation (2022B1515020092). We also acknowledge the Fundamental Research Funds for the Central Universities (Nos. D5000210283, D5000210601, and D5000210829). The calculations were supported by TianHe-2 at Shanxi Supercomputing Center of China and Central for High Performance Computing of Northwestern Polytechnical University.

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