Micropore-confined Ru nanoclusters catalyst for efficient pH-universal hydrogen evolution reaction

Xiaoxiao Huang; Ruihu Lu; Yaping Cen; Dunchao Wang; Shao Jin; Wenxing Chen; Geoffrey I.; N. Waterhouse; Ziyun Wang; Shubo Tian; Xiaoming Sun

doi:10.1007/s12274-023-5711-1

Nano Research 2023, 16(7): 9073-9080 https://doi.org/10.1007/s12274-023-5711-1

Research Article | Issue | Published: 25 May 2023

Micropore-confined Ru nanoclusters catalyst for efficient pH-universal hydrogen evolution reaction

Show Author's Information Hide Author's Information Xiaoxiao Huang^{¹^,^§}, Ruihu Lu^{²^,^§}, Yaping Cen^¹, Dunchao Wang^¹, Shao Jin^¹, Wenxing Chen^³, Geoffrey I.^{¹^,²^,³}, N. Waterhouse^², Ziyun Wang^²(

), Shubo Tian^¹(

), Xiaoming Sun^¹(

)

1State Key Laboratory of Chemical Resource Engineering College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China

2School of Chemical Sciences, The University of Auckland, Auckland 1010, New Zealand

3School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

^§ Xiaoxiao Huang and Ruihu Lu contributed equally to this work.

Keywords:

hydrogen evolution reaction, Ru nanoparticles, Ru nanoclusters, Ru single atoms

Topics:

Hydrogen evolution reaction Nanoclusters

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Huang X, Lu R, Cen Y, et al. Micropore-confined Ru nanoclusters catalyst for efficient pH-universal hydrogen evolution reaction. Nano Research, 2023, 16(7): 9073-9080. https://doi.org/10.1007/s12274-023-5711-1

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Abstract Full text Electronic supplementary material About this article

Abstract

Pt-based catalysts are used commercially for the hydrogen evolution reaction (HER), even though the low earth abundance and high cost of platinum hinder scale-up applications. Ru metal is a promising alternative catalyst for HER owing to its lower cost but similar metal–hydrogen bond strength to Pt. However, designing an efficient and robust Ru-based electrocatalyst for pH-universal HER is challenging. Herein, we successfully synthesized N-doped carbon (NC) supported ruthenium catalysts with different Ru sizes (single-atoms, nanoclusters and nanoparticles), and then systematically evaluated their performance for HER. Among these catalysts, the Ru nanocluster catalyst (Ru NCs/NC) displayed optimal catalytic performance with overpotentials of only 14, 30, and 32 mV (at 10 mA·cm⁻²) in 1 M KOH, 1 M phosphate buffer saline (PBS), and 0.5 M H₂SO₄, respectively. The corresponding mass activities were 32.2, 12.1 and 8.1 times higher than those of 20 wt.% Pt/C, and also much better than those of the Ru single-atoms (Ru SAs/NC) and Ru nanoparticle (Ru NPs/NC) catalysts, at an overpotential of 100 mV under alkaline, neutral and acidic conditions, respectively. Density functional theory (DFT) calculations revealed that the outstanding HER performance of the Ru NCs/NC catalyst resulted from a strong interaction between the Ru nanoclusters and the N-doped carbon support, which downshifted the d-band center and thus weakened the *H adsorption ability of Ru sites.

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Micropore-confined Ru nanoclusters catalyst for efficient pH-universal hydrogen evolution reaction

Show Author's information Hide Author's Information Xiaoxiao Huang^{¹^,^§}, Ruihu Lu^{²^,^§}, Yaping Cen^¹, Dunchao Wang^¹, Shao Jin^¹, Wenxing Chen^³, Geoffrey I.^{¹^,²^,³}, N. Waterhouse^², Ziyun Wang^²(

), Shubo Tian^¹(

), Xiaoming Sun^¹(

)

1State Key Laboratory of Chemical Resource Engineering College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China

2School of Chemical Sciences, The University of Auckland, Auckland 1010, New Zealand

3School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

^§ Xiaoxiao Huang and Ruihu Lu contributed equally to this work.

Abstract

Keywords: hydrogen evolution reaction, Ru nanoparticles, Ru nanoclusters, Ru single atoms

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Acknowledgements

Publication history

Received: 20 February 2023

Revised: 03 April 2023

Accepted: 07 April 2023

Published: 25 May 2023

Issue date: July 2023

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Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (Nos. 2021YFA1502200 and 2022YFA1504003), the National Natural Science Foundation of China (Nos. 21935001 and 22101015), and the Fundamental Research Funds of Beijing University of Chemical Technology (Nos. buctrc202107 and buctrc202212). The computational study was supported by the Marsden Fund Council (No. 21-UOA-237) from Government funding, managed by Royal Society Te Apārangi and Catalyst: Seeding Grant (22-UOA-031-CSG) provided by the New Zealand Ministry of Business, Innovation and Employment and administered by the Royal Society Te Apārangi. Z. Y. W. and R. H. L. wish to acknowledge the use of New Zealand eScience Infrastructure (NeSI) high performance computing facilities, consulting support, and/or training services as part of this research. GINW acknowledges funding support from the Royal Society Te Apārangi (for the award of James Cook Research Fellowship).