Densely populated trimetallic single-atoms for durable low-temperature flexible zinc-air batteries

• Published in: Applied catalysis. B, Environmental Vol. 342; p. 123438
• Main Authors: Zhai, Wenfang, He, Yuting, Duan, Yu-e, Guo, Shengwu, Chen, Yuanzhen, Dai, Zhengfei, Liu, Liting, Tan, Qiang
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.03.2024
• Subjects: Bifunctional oxygen electrocatalyst; Flexible Zn-air battery; Heteroatom coordination; Trimetallic single-atoms; Heteroatom coordination; Bifunctional oxygen electrocatalyst; Flexible Zn-air battery; Trimetallic single-atoms
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.123438

The fundamental challenge of trimetallic single-atoms catalysts stems from the difficulty in supporting the coexistence of different metals with their unique physicochemical features. Here, the trimetallic single-atoms electrocatalyst is constructed as a model system to explore electrocatalytic ORR/OER. The tri-metal (Fe, Co, and Ni) single-atoms loaded on nitrogen-carbon framework exhibits superior ORR/OER kinetics (E1/2 = 0.927 V, Ej=10 = 1.56 V). The flexible zinc-air batteries generate excellent power density and durability (62 mW cm−2 and 200 h at −15 °C, 291.2 mW cm−2 and 250 h at room temperature). Density functional calculations confirm that the trimetallic synergy effect outperform mono- and bimetallic effects, yielding adsorption strength close to 0. This paper describes an intuitionistic descriptor where ΔEOH* displays a volcano relationship with ORR overpotential, and establishes a generalized strategy for efficient bifunctional oxygen electrocatalyst while comprehensively understanding the structure-mechanism-activity relationship. [Display omitted] •Tri-metal incorporated nitrogen-carbon catalysts possesses high density and well dispersed tri-metal single atom sites.•Fe3%Co3%Ni9%-NC1000 display outstanding ORR/OER performance.•The descriptor ΔEOH* displays a volcano relationship with ORR overpotential.•Flexible zinc-air batteries assembled with Fe3%Co3%Ni9%-NC1000 generate superior power density and durability.