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Nano Research https://doi.org/10.1007/s12274-024-6528-2
Research Article | Online first | Published: 03 April 2024

Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

Show Author's Information Yuwei He1,  Yueguang Chen1( ),  Renjie Wu1,  Zhihe Xiao1,  Mengxian Li1,  Chunfeng Shi2( ),  Leyu Wang1( )
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
State Key Laboratory of Petroleum Molecular and Process Engineering, SINOPEC Research Institute of Petroleum Processing Co., Beijing 100083, China
Keywords:
oxygen reduction reaction, ultrathin nanowires, ligand effect, group VI B transition metal, multiple oxygen species
Topics:
Oxygen evolution reactionProton exchange membrane fuel cells (PEMFC) Structural optimization
Cite this article:
He Y, Chen Y, Wu R, et al. Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6528-2
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Abstract Full text Electronic supplementary material About this article

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells (PEMFCs). Despite extensive research on catalysts for the cathodic oxygen reduction reaction (ORR), developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains challenging. Herein, we report a facile synthesis of bimetallic ultrathin PtM (M = Mo, W, and Cr) nanowires (NWs) composed of group VI B transition metal atomic sites anchored on the surface. These NWs possess uniform sizes and well-controlled atomic arrangements. Compared to PtW and PtCr catalysts, the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt−1. Remarkably, they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR, surpassing previously reported Pt-based catalysts. Additionally, the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm−2 (H2-O2 conditions at 80 °C), which is 1.09 times that of commercial Pt/C. The ligand effect in the bimetallic surface not only facilitates strong coupling between Mo (4d) and Pt (5d) atomic orbitals to hinder atom leaching but also modulates the d-states of active site, significantly optimizing the adsorption of key oxygen (*O and *OH) species and accelerating the rate-determining step in ORR pathways.


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About this article

Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

Show Author's information Yuwei He1, Yueguang Chen1( ), Renjie Wu1, Zhihe Xiao1, Mengxian Li1, Chunfeng Shi2( ), Leyu Wang1( )
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
State Key Laboratory of Petroleum Molecular and Process Engineering, SINOPEC Research Institute of Petroleum Processing Co., Beijing 100083, China

Abstract

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells (PEMFCs). Despite extensive research on catalysts for the cathodic oxygen reduction reaction (ORR), developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains challenging. Herein, we report a facile synthesis of bimetallic ultrathin PtM (M = Mo, W, and Cr) nanowires (NWs) composed of group VI B transition metal atomic sites anchored on the surface. These NWs possess uniform sizes and well-controlled atomic arrangements. Compared to PtW and PtCr catalysts, the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt−1. Remarkably, they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR, surpassing previously reported Pt-based catalysts. Additionally, the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm−2 (H2-O2 conditions at 80 °C), which is 1.09 times that of commercial Pt/C. The ligand effect in the bimetallic surface not only facilitates strong coupling between Mo (4d) and Pt (5d) atomic orbitals to hinder atom leaching but also modulates the d-states of active site, significantly optimizing the adsorption of key oxygen (*O and *OH) species and accelerating the rate-determining step in ORR pathways.

Keywords: oxygen reduction reaction, ultrathin nanowires, ligand effect, group VI B transition metal, multiple oxygen species

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Publication history
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Acknowledgements

Publication history

Received: 27 December 2023
Revised: 29 January 2024
Accepted: 30 January 2024
Published: 03 April 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This research was supported by the National Natural Science Foundation of China (No. 22275009), SINOPEC (contact No. 421028), and Fundamental Research Funds for the Central Universities (No. XK2020-02). We thank the BL14W1 station in Shanghai Synchrotron Radiation Facility (SSRF). The authors would like to express their gratitude to Prof. Zhongbin Zhuang, Prof. Wei Zhu, and Mr. Chengjin Chen from BUCT for their assistance with the MEA test.

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