Electron Localization in Rationally Designed Pt1Pd Single-Atom Alloy Catalyst Enables High-Performance Li-O2 Batteries

Erhuan Zhang; Anqi Dong; Kun Yin; Chenliang Ye; Yin Zhou; Chuan Tan; Menggang Li; Xiaobo Zheng; Yu Wang; Xiangwen Gao; Hongbo Li; Dingsheng Wang; Shaojun Guo

doi:10.1021/jacs.3c12734

Electron Localization in Rationally Designed Pt₁Pd Single-Atom Alloy Catalyst Enables High-Performance Li-O₂ Batteries

J Am Chem Soc. 2024 Jan 31;146(4):2339-2344. doi: 10.1021/jacs.3c12734. Epub 2024 Jan 18.

Authors

Erhuan Zhang¹, Anqi Dong², Kun Yin^{3

4}, Chenliang Ye⁵, Yin Zhou³, Chuan Tan¹, Menggang Li³, Xiaobo Zheng⁶, Yu Wang⁷, Xiangwen Gao¹, Hongbo Li⁴, Dingsheng Wang⁶, Shaojun Guo³

Affiliations

¹ Future Battery Research Center, Global Institute of Future Technology, Shanghai Jiao Tong University, Shanghai 200240, China.
² School of Materials Science & Engineering, Anhui University, Hefei 230601, China.
³ School of Materials Science and Engineering, Peking University, Beijing 100871, China.
⁴ Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China.
⁵ Department of Power Engineering, North China Electric Power University, Baoding 071003, Hebei, China.
⁶ Department of Chemistry, Tsinghua University, Beijing 100084, China.
⁷ Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China.

PMID: 38237055
DOI: 10.1021/jacs.3c12734

Abstract

Li-O₂ batteries (LOBs) are considered as one of the most promising energy storage devices due to their ultrahigh theoretical energy density, yet they face the critical issues of sluggish cathode redox kinetics during the discharge and charge processes. Here we report a direct synthetic strategy to fabricate a single-atom alloy catalyst in which single-atom Pt is precisely dispersed in ultrathin Pd hexagonal nanoplates (Pt₁Pd). The LOB with the Pt₁Pd cathode demonstrates an ultralow overpotential of 0.69 V at 0.5 A g^-1 and negligible activity loss over 600 h. Density functional theory calculations show that Pt₁Pd can promote the activation of the O₂/Li₂O₂ redox couple due to the electron localization caused by the single Pt atom, thereby lowering the energy barriers for the oxygen reduction and oxygen evolution reactions. Our strategy for designing single-atom alloy cathodic catalysts can address the sluggish oxygen redox kinetics in LOBs and other energy storage/conversion devices.