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Nano Research 2023, 16(7): 9012-9021 https://doi.org/10.1007/s12274-023-5667-1
Research Article | Issue | Published: 24 April 2023

Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation

Show Author's Information Xinru Zhao1,  Yanyan Liu1,2,  Huiyu Yuan3,  Hao Wen4,  Huanhuan Zhang1,4,  Saima Ashraf4,  Shuyan Guan1,4,  Tao Liu5,  Sehrish Mehdi4,  Ruofan Shen4,  Xianji Guo4,  Yanping Fan1,  Baozhong Liu1,6( ),  Baojun Li1,4,7( )
College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo 454000, China
College of Science, Henan Agriculture University, Zhengzhou 450002, China
College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University, Zhengzhou 450001, China
CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, National Centre for Nanoscience and Technology, Beijing 100190, China
State Collaborative Innovation Center of Coal Work Safety and Clean-efficiency Utilization, Jiaozuo 454003, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Keywords:
dual-active sites, PdCu nanoalloy, d-band holes, borohydride hydrolysis, ensemble effect
Topics:
Catalysis Catalyst activity
Cite this article:
Zhao X, Liu Y, Yuan H, et al. Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation. Nano Research, 2023, 16(7): 9012-9021. https://doi.org/10.1007/s12274-023-5667-1
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Abstract Full text Electronic supplementary material About this article

The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO2 encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279 mol H2∙min−1∙molPd−1) ranking the third place among Pd-based catalysts was achieved in the absence of alkali. Both experimental research and theoretical calculations reveal a lower activation energy of the B–H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O–H bond than that on pristine Cu. The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd0.1Cu0.9/TiO2-porous carbon (Pd0.1Cu0.9/T-PC). This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis.


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Abstract
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Electronic supplementary material
About this article

Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation

Show Author's information Xinru Zhao1, Yanyan Liu1,2, Huiyu Yuan3, Hao Wen4, Huanhuan Zhang1,4, Saima Ashraf4, Shuyan Guan1,4, Tao Liu5, Sehrish Mehdi4, Ruofan Shen4, Xianji Guo4, Yanping Fan1, Baozhong Liu1,6( ), Baojun Li1,4,7( )
College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo 454000, China
College of Science, Henan Agriculture University, Zhengzhou 450002, China
College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University, Zhengzhou 450001, China
CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, National Centre for Nanoscience and Technology, Beijing 100190, China
State Collaborative Innovation Center of Coal Work Safety and Clean-efficiency Utilization, Jiaozuo 454003, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

Abstract

The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO2 encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279 mol H2∙min−1∙molPd−1) ranking the third place among Pd-based catalysts was achieved in the absence of alkali. Both experimental research and theoretical calculations reveal a lower activation energy of the B–H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O–H bond than that on pristine Cu. The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd0.1Cu0.9/TiO2-porous carbon (Pd0.1Cu0.9/T-PC). This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis.

Keywords: dual-active sites, PdCu nanoalloy, d-band holes, borohydride hydrolysis, ensemble effect

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Publication history
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Acknowledgements

Publication history

Received: 06 February 2023
Revised: 09 March 2023
Accepted: 12 March 2023
Published: 24 April 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22279118, 22279117, 52071135, 51871090, and U1804135) and the Fundamental Research Funds for the Universities of Henan Province (No. NSFRF220201).

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