A Tensile-Strained Pt-Rh Single-Atom Alloy Remarkably Boosts Ethanol Oxidation

Shuiping Luo; Long Zhang; Yujia Liao; Lanxi Li; Qi Yang; Xiaotong Wu; Xiaoyu Wu; Dongsheng He; Chunyong He; Wen Chen; Qilong Wu; Mingrui Li; Emiel J M Hensen; Zewei Quan

doi:10.1002/adma.202008508

A Tensile-Strained Pt-Rh Single-Atom Alloy Remarkably Boosts Ethanol Oxidation

Adv Mater. 2021 Apr;33(17):e2008508. doi: 10.1002/adma.202008508. Epub 2021 Mar 22.

Authors

Shuiping Luo¹, Long Zhang², Yujia Liao¹, Lanxi Li¹, Qi Yang¹, Xiaotong Wu¹, Xiaoyu Wu¹, Dongsheng He³, Chunyong He⁴, Wen Chen¹, Qilong Wu¹, Mingrui Li¹, Emiel J M Hensen², Zewei Quan¹

Affiliations

¹ Department of Chemistry, Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Shenzhen Engineering Research Center for Frontier Materials Synthesis at High Pressures, Southern University of Science and Technology (SUSTech), Shenzhen, Guangdong, 518055, P. R. China.
² Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P. O. Box 513, Eindhoven, MB, 5600, The Netherlands.
³ Materials Characterization and Preparation Center (MCPC), Southern University of Science and Technology (SUSTech), Shenzhen, Guangdong, 518055, P. R. China.
⁴ Spallation Neutron Source Science Center, Dongguan, 523803, P. R. China.

PMID: 33749954
DOI: 10.1002/adma.202008508

Abstract

The rational design and control of electrocatalysts at single-atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi-Rh₁ ) by atomic galvanic replacement, and their subsequent transformation into a tensile-strained Pt-Rh single-atom alloy (PtBi@PtRh₁ ) via electrochemical dealloying are presented. Benefiting from the Rh₁ -tailored Pt (110) surface with tensile strain, the PtBi@PtRh₁ nanoplates exhibit record-high and all-round superior electrocatalytic performance including activity, selectivity, stability, and anti-poisoning ability toward ethanol oxidation in alkaline electrolytes. Density functional theory calculations reveal the synergism between effective Rh₁ and tensile strain in boosting the adsorption of ethanol and key surface intermediates and the CC bond cleavage of the intermediates. The facile synthesis of the tensile-strained single-atom alloy provides a novel strategy to construct model nanostructures, accelerating the development of highly efficient electrocatalysts.

Keywords: electrocatalysis; ethanol oxidation; intermetallics; single-atom alloys; strain effect.

Abstract

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