Platinum-Ruthenium Single Atom Alloy as a Bifunctional Electrocatalyst toward Methanol and Hydrogen Oxidation Reactions

Ligang Chen; Xin Liang; Dingsheng Wang; Zuobo Yang; Chun Ting He; Wei Zhao; Jiajing Pei; Yanrong Xue

doi:10.1021/acsami.2c02905

Platinum-Ruthenium Single Atom Alloy as a Bifunctional Electrocatalyst toward Methanol and Hydrogen Oxidation Reactions

Ligang Chen, Xin Liang^*, Dingsheng Wang, Zuobo Yang, Chun Ting He, Wei Zhao, Jiajing Pei, Yanrong Xue

^*Corresponding author for this work

Physical Sciences and Engineering

Research output: Contribution to journal › Article › peer-review

27 Scopus citations

Abstract

The precise regulation for the structural properties of nanomaterials at the atomic scale is an effective strategy to develop high-performance catalysts. Herein, a facile dual-regulation approach was developed to successfully synthesize Ru₁Pt_nsingle atom alloy (SAA) with atomic Ru dispersed in Pt nanocrystals. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure demonstrated that Ru atoms were dispersed in Pt nanocrystals as single atoms. Impressively, the Ru₁Pt_n-SAA exhibited an ultrahigh specific activity (23.59 mA cm^-2) and mass activity (2.805 mA/μg_-PtRu) for methanol oxidation reaction (MOR) and exhibited excellent exchange current density activity (1.992 mA cm^-2) and mass activity (4.71 mA/μg_-PtRu) for hydrogen oxidation reaction (HOR). Density functional theory calculations revealed that the introduction of Ru atoms greatly reduced the reaction free energy for the decomposition of water molecules, which promoted the removal of CO∗ in the MOR process and adjusted the Gibbs free energy of hydrogen and hydroxyl adsorption to promote the HOR. Our work provided an effective idea for the development of high performance electrocatalysts.

Original language	English (US)
Pages (from-to)	27814-27822
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	14
Issue number	24
DOIs	https://doi.org/10.1021/acsami.2c02905
State	Published - Jun 22 2022

Bibliographical note

Funding Information:
This work was supported by the National Key R&D Program of China (Grant 2018YFA0702000). C.-T.H. acknowledges the support of the Jiangxi Provincial Department of Science and Technology (Grant 20202ZDB01004). We thank the 1W1B station for XAFS measurements at Beijing Synchrotron Radiation Facility (BSRF) and the BL14W1 station for XAFS measurements at Shanghai Synchrotron Radiation Facility (SSRF).

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

Keywords

electrocatalyst
hydrogen oxidation reaction
methanol oxidation reaction
platinum nanocrystals
single atom alloy

ASJC Scopus subject areas

General Materials Science

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10.1021/acsami.2c02905

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title = "Platinum-Ruthenium Single Atom Alloy as a Bifunctional Electrocatalyst toward Methanol and Hydrogen Oxidation Reactions",

abstract = "The precise regulation for the structural properties of nanomaterials at the atomic scale is an effective strategy to develop high-performance catalysts. Herein, a facile dual-regulation approach was developed to successfully synthesize Ru1Ptnsingle atom alloy (SAA) with atomic Ru dispersed in Pt nanocrystals. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure demonstrated that Ru atoms were dispersed in Pt nanocrystals as single atoms. Impressively, the Ru1Ptn-SAA exhibited an ultrahigh specific activity (23.59 mA cm-2) and mass activity (2.805 mA/μg-PtRu) for methanol oxidation reaction (MOR) and exhibited excellent exchange current density activity (1.992 mA cm-2) and mass activity (4.71 mA/μg-PtRu) for hydrogen oxidation reaction (HOR). Density functional theory calculations revealed that the introduction of Ru atoms greatly reduced the reaction free energy for the decomposition of water molecules, which promoted the removal of CO∗ in the MOR process and adjusted the Gibbs free energy of hydrogen and hydroxyl adsorption to promote the HOR. Our work provided an effective idea for the development of high performance electrocatalysts.",

keywords = "electrocatalyst, hydrogen oxidation reaction, methanol oxidation reaction, platinum nanocrystals, single atom alloy",

author = "Ligang Chen and Xin Liang and Dingsheng Wang and Zuobo Yang and He, {Chun Ting} and Wei Zhao and Jiajing Pei and Yanrong Xue",

note = "Funding Information: This work was supported by the National Key R&D Program of China (Grant 2018YFA0702000). C.-T.H. acknowledges the support of the Jiangxi Provincial Department of Science and Technology (Grant 20202ZDB01004). We thank the 1W1B station for XAFS measurements at Beijing Synchrotron Radiation Facility (BSRF) and the BL14W1 station for XAFS measurements at Shanghai Synchrotron Radiation Facility (SSRF). Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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AU - Chen, Ligang

AU - Liang, Xin

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AU - Yang, Zuobo

AU - He, Chun Ting

AU - Zhao, Wei

AU - Pei, Jiajing

AU - Xue, Yanrong

N1 - Funding Information: This work was supported by the National Key R&D Program of China (Grant 2018YFA0702000). C.-T.H. acknowledges the support of the Jiangxi Provincial Department of Science and Technology (Grant 20202ZDB01004). We thank the 1W1B station for XAFS measurements at Beijing Synchrotron Radiation Facility (BSRF) and the BL14W1 station for XAFS measurements at Shanghai Synchrotron Radiation Facility (SSRF). Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/6/22

Y1 - 2022/6/22

N2 - The precise regulation for the structural properties of nanomaterials at the atomic scale is an effective strategy to develop high-performance catalysts. Herein, a facile dual-regulation approach was developed to successfully synthesize Ru1Ptnsingle atom alloy (SAA) with atomic Ru dispersed in Pt nanocrystals. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure demonstrated that Ru atoms were dispersed in Pt nanocrystals as single atoms. Impressively, the Ru1Ptn-SAA exhibited an ultrahigh specific activity (23.59 mA cm-2) and mass activity (2.805 mA/μg-PtRu) for methanol oxidation reaction (MOR) and exhibited excellent exchange current density activity (1.992 mA cm-2) and mass activity (4.71 mA/μg-PtRu) for hydrogen oxidation reaction (HOR). Density functional theory calculations revealed that the introduction of Ru atoms greatly reduced the reaction free energy for the decomposition of water molecules, which promoted the removal of CO∗ in the MOR process and adjusted the Gibbs free energy of hydrogen and hydroxyl adsorption to promote the HOR. Our work provided an effective idea for the development of high performance electrocatalysts.

AB - The precise regulation for the structural properties of nanomaterials at the atomic scale is an effective strategy to develop high-performance catalysts. Herein, a facile dual-regulation approach was developed to successfully synthesize Ru1Ptnsingle atom alloy (SAA) with atomic Ru dispersed in Pt nanocrystals. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure demonstrated that Ru atoms were dispersed in Pt nanocrystals as single atoms. Impressively, the Ru1Ptn-SAA exhibited an ultrahigh specific activity (23.59 mA cm-2) and mass activity (2.805 mA/μg-PtRu) for methanol oxidation reaction (MOR) and exhibited excellent exchange current density activity (1.992 mA cm-2) and mass activity (4.71 mA/μg-PtRu) for hydrogen oxidation reaction (HOR). Density functional theory calculations revealed that the introduction of Ru atoms greatly reduced the reaction free energy for the decomposition of water molecules, which promoted the removal of CO∗ in the MOR process and adjusted the Gibbs free energy of hydrogen and hydroxyl adsorption to promote the HOR. Our work provided an effective idea for the development of high performance electrocatalysts.

KW - electrocatalyst

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KW - methanol oxidation reaction

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ER -

Platinum-Ruthenium Single Atom Alloy as a Bifunctional Electrocatalyst toward Methanol and Hydrogen Oxidation Reactions

Abstract

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Keywords

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