Maximizing the Catalytic Performance of Pd@AuxPd1−x Nanocubes in H2O2 Production by Reducing Shell Thickness to Increase Compositional Stability

Yu Zhang; Zhiheng Lyu; Zitao Chen; Shangqian Zhu; Yifeng Shi; Ruhui Chen; Minghao Xie; Yao Yao; Miaofang Chi; Minhua Shao; Younan Xia

doi:10.1002/anie.202105137

Maximizing the Catalytic Performance of Pd@Au_xPd_1−x Nanocubes in H₂O₂ Production by Reducing Shell Thickness to Increase Compositional Stability

Yu Zhang, Zhiheng Lyu, Zitao Chen, Shangqian Zhu, Yifeng Shi, Ruhui Chen, Minghao Xie, Yao Yao, Miaofang Chi, Minhua Shao, Younan Xia

electron Microscopy and Microanalysis

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

50 Scopus citations

Abstract

We report a simple route based upon seed-mediated growth to the synthesis of Pd@Au_xPd_1−x (0.8≤x≤1) core–shell nanocubes. Benefiting from the well-defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au_0.95Pd_0.05 work as an efficient electrocatalyst toward H₂O₂ production, with high selectivity of 93–100 % in the low-overpotential region of 0.4–0.7 V. When the Au_0.95Pd_0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H₂O₂ during oxygen reduction at a high rate of 1.62 mol g_(Pd+Au)⁻¹ h⁻¹. This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals.

Original language	English
Pages (from-to)	19643-19647
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	36
DOIs	https://doi.org/10.1002/anie.202105137
State	Published - Sep 1 2021

Funding

This work was supported in part by start‐up funds from the Georgia Institute of Technology. Part of the electron microscopy work was performed through a user project supported by the ORNL′s Center for Nanophase Materials Sciences, which is a U.S. Department of Energy Office of Science User Facility. This work was also supported by the Research Grant Council (Project No. HKUST C6011‐20G) of the Hong Kong Special Administrative Region and Hong Kong Branch of Southern Marine Science and Engineering Guangdong Laboratory (SMSEGL20SC01).

Funders	Funder number
Hong Kong Special Administrative Region and Hong Kong Branch of Southern Marine Science and Engineering Guangdong Laboratory	SMSEGL20SC01
ORNL′s Center for Nanophase Materials Sciences
Office of Science
Georgia Institute of Technology
Research Grants Council, University Grants Committee

Keywords

alloys
electrocatalysts
noble metals
shell
surface stability

Access to Document

10.1002/anie.202105137

Cite this

@article{4cfc6a5d04f54e5e9021bd4e0b0450ed,

title = "Maximizing the Catalytic Performance of Pd@AuxPd1−x Nanocubes in H2O2 Production by Reducing Shell Thickness to Increase Compositional Stability",

abstract = "We report a simple route based upon seed-mediated growth to the synthesis of Pd@AuxPd1−x (0.8≤x≤1) core–shell nanocubes. Benefiting from the well-defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au0.95Pd0.05 work as an efficient electrocatalyst toward H2O2 production, with high selectivity of 93–100 % in the low-overpotential region of 0.4–0.7 V. When the Au0.95Pd0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H2O2 during oxygen reduction at a high rate of 1.62 mol g(Pd+Au)−1 h−1. This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals.",

keywords = "alloys, electrocatalysts, noble metals, shell, surface stability",

author = "Yu Zhang and Zhiheng Lyu and Zitao Chen and Shangqian Zhu and Yifeng Shi and Ruhui Chen and Minghao Xie and Yao Yao and Miaofang Chi and Minhua Shao and Younan Xia",

note = "Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

month = sep,

day = "1",

doi = "10.1002/anie.202105137",

language = "English",

volume = "60",

pages = "19643--19647",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "wiley",

number = "36",

}

TY - JOUR

T1 - Maximizing the Catalytic Performance of Pd@AuxPd1−x Nanocubes in H2O2 Production by Reducing Shell Thickness to Increase Compositional Stability

AU - Zhang, Yu

AU - Lyu, Zhiheng

AU - Chen, Zitao

AU - Zhu, Shangqian

AU - Shi, Yifeng

AU - Chen, Ruhui

AU - Xie, Minghao

AU - Yao, Yao

AU - Chi, Miaofang

AU - Shao, Minhua

AU - Xia, Younan

PY - 2021/9/1

Y1 - 2021/9/1

N2 - We report a simple route based upon seed-mediated growth to the synthesis of Pd@AuxPd1−x (0.8≤x≤1) core–shell nanocubes. Benefiting from the well-defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au0.95Pd0.05 work as an efficient electrocatalyst toward H2O2 production, with high selectivity of 93–100 % in the low-overpotential region of 0.4–0.7 V. When the Au0.95Pd0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H2O2 during oxygen reduction at a high rate of 1.62 mol g(Pd+Au)−1 h−1. This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals.

AB - We report a simple route based upon seed-mediated growth to the synthesis of Pd@AuxPd1−x (0.8≤x≤1) core–shell nanocubes. Benefiting from the well-defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au0.95Pd0.05 work as an efficient electrocatalyst toward H2O2 production, with high selectivity of 93–100 % in the low-overpotential region of 0.4–0.7 V. When the Au0.95Pd0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H2O2 during oxygen reduction at a high rate of 1.62 mol g(Pd+Au)−1 h−1. This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals.

KW - alloys

KW - electrocatalysts

KW - noble metals

KW - shell

KW - surface stability

UR - http://www.scopus.com/inward/record.url?scp=85111653149&partnerID=8YFLogxK

U2 - 10.1002/anie.202105137

DO - 10.1002/anie.202105137

M3 - Article

C2 - 34128305

AN - SCOPUS:85111653149

SN - 1433-7851

VL - 60

SP - 19643

EP - 19647

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 36

ER -