Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis

Lin He; Menggang Li; Longyu Qiu; Shuo Geng; Yequn Liu; Fenyang Tian; Mingchuan Luo; Hu Liu; Yongsheng Yu; Weiwei Yang; Shaojun Guo

doi:10.1038/s41467-024-45874-z

Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis

Nat Commun. 2024 Mar 13;15(1):2290. doi: 10.1038/s41467-024-45874-z.

Authors

Lin He^#¹, Menggang Li^#^{1

2}, Longyu Qiu^#¹, Shuo Geng³, Yequn Liu⁴, Fenyang Tian¹, Mingchuan Luo², Hu Liu⁵, Yongsheng Yu⁶, Weiwei Yang⁷, Shaojun Guo⁸

Affiliations

¹ State Key Laboratory of Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, 150001, China.
² School of Materials Science and Engineering, Peking University, Beijing, 100871, China.
³ Department of Chemical Engineering, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, 550025, China.
⁴ Analytical Instrumentation Center, State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.
⁵ Key Laboratory of Green and High-end Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining, 810008, China.
⁶ State Key Laboratory of Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, 150001, China. ysyu@hit.edu.cn.
⁷ State Key Laboratory of Urban Water Resource and Environment, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, 150001, China. yangww@hit.edu.cn.
⁸ School of Materials Science and Engineering, Peking University, Beijing, 100871, China. guosj@pku.edu.cn.

^# Contributed equally.

Abstract

The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing for energy conversion, yet remains a grand challenge. Herein, we report a class of single-atom Mo-tailored PdPtNiCuZn high-entropy-alloy nanosheets with dilute Pt-Pt ensembles and intrinsic tensile strain (Mo₁-PdPtNiCuZn) as efficient electrocatalysts for enhancing the methanol oxidation reaction catalysis. The as-made Mo₁-PdPtNiCuZn delivers an extraordinary mass activity of 24.55 A mg_Pt^-1 and 11.62 A mg_Pd+Pt^-1, along with impressive long-term durability. The planted oxophilic Mo single atoms as promoters modify the electronic structure of isolated Pt sites in the high-entropy-alloy host, suppressing the formation of CO adsorbates and steering the reaction towards the formate pathway. Meanwhile, Mo promoters and tensile strain synergistically optimize the adsorption behaviour of intermediates to achieve a more energetically favourable pathway and minimize the methanol oxidation reaction barrier. This work advances the design of atomically precise catalytic sites by creating a new paradigm of single atom-tailored high-entropy alloys, opening an encouraging pathway to the design of CO-tolerance electrocatalysts.

Abstract

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