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Nano Research 2021, 14(8): 2659-2665 https://doi.org/10.1007/s12274-020-3269-8
Research Article | Issue | Published: 28 December 2020

Suppressing the surface passivation of Pt-Mo nanowires via constructing Mo-Se coordination for boosting HER performance

Show Author's Information Lei Yu1,  Tingting Zhou1,  Shuhua Cao1,  Xishi Tai1,  Lili Liu1,  Yao Wang2( )
School of Chemistry & Chemical Engineering and Environmental Engineering, Weifang University, Weifang 261061, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Keywords:
hydrogen evolution reaction, Pt based alloys, electron effect, interfacial synergy, water dissociation
Topics:
Binary alloysDensity functional theoryHydrogenHydrogen evolution reaction NanocrystalsNanowiresPlatinum metalsSeleniumSurface structureTransition metalsX-ray photoelectron spectroscopy
Cite this article:
Yu L, Zhou T, Cao S, et al. Suppressing the surface passivation of Pt-Mo nanowires via constructing Mo-Se coordination for boosting HER performance. Nano Research, 2021, 14(8): 2659-2665. https://doi.org/10.1007/s12274-020-3269-8
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Abstract Full text Electronic supplementary material About this article

Modulating the surface coordination environment of Pt based nanocrystals at the atomic level is of great importance to obtain good electrocatalytic performance. Given the fundamental understandings of surface structure degeneration of Pt based nanocrystals, introducing a weak electronegative element to the surface of Pt-based catalysts is beneficial for suppressing surface passivation and improving hydrogen evolution reaction performance of Pt. Density functional theory results reveal that the energy barrier of water dissociation process can be greatly reduced by using Se element as the surface modifier to replace the O. This hypothesis is further validated by experiments that ultralong Pt85Mo15-Se nanowires were fabricated to suppress the excessive passivation behavior of transition metals of Pt based alloy. The Pt85Mo15-Se nanowires exhibit higher activity with 4.98 times the specific activity and 4.87 times the mass activity of commercial Pt/C, as well as a better stability towards alkaline hydrogen evolution reaction. The deep exploration of X-ray photoelectron spectroscopy and theoretical calculations disclose that Se element could maintain the electron-rich state around the electronic orbit of Pt. This study provides a new insight to advance the fundamental understanding on electrocatalytic materials, which exhibits a promising approach to protect the surface chemical environment of Pt based nanocrystals.


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Electronic supplementary material
About this article

Suppressing the surface passivation of Pt-Mo nanowires via constructing Mo-Se coordination for boosting HER performance

Show Author's information Lei Yu1, Tingting Zhou1, Shuhua Cao1, Xishi Tai1, Lili Liu1, Yao Wang2( )
School of Chemistry & Chemical Engineering and Environmental Engineering, Weifang University, Weifang 261061, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

Abstract

Modulating the surface coordination environment of Pt based nanocrystals at the atomic level is of great importance to obtain good electrocatalytic performance. Given the fundamental understandings of surface structure degeneration of Pt based nanocrystals, introducing a weak electronegative element to the surface of Pt-based catalysts is beneficial for suppressing surface passivation and improving hydrogen evolution reaction performance of Pt. Density functional theory results reveal that the energy barrier of water dissociation process can be greatly reduced by using Se element as the surface modifier to replace the O. This hypothesis is further validated by experiments that ultralong Pt85Mo15-Se nanowires were fabricated to suppress the excessive passivation behavior of transition metals of Pt based alloy. The Pt85Mo15-Se nanowires exhibit higher activity with 4.98 times the specific activity and 4.87 times the mass activity of commercial Pt/C, as well as a better stability towards alkaline hydrogen evolution reaction. The deep exploration of X-ray photoelectron spectroscopy and theoretical calculations disclose that Se element could maintain the electron-rich state around the electronic orbit of Pt. This study provides a new insight to advance the fundamental understanding on electrocatalytic materials, which exhibits a promising approach to protect the surface chemical environment of Pt based nanocrystals.

Keywords: hydrogen evolution reaction, Pt based alloys, electron effect, interfacial synergy, water dissociation

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Publication history
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Acknowledgements

Publication history

Received: 07 September 2020
Revised: 19 October 2020
Accepted: 29 October 2020
Published: 28 December 2020
Issue date: August 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

Acknowledgements

The authors gratefully acknowledge the Science Foundation of Weifang University (No. 2020BS16), the Natural Science Foundation of Shandong Province (No. ZR2019BEM017 and ZR2017MB056), and the financial support of the National Natural Science Foundation of China (No. 21802104).

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