Ternary Synergism of Heterogeneous M1N4‐C‐M2N4‐C‐M3N4 Single‐Atom Sites to Manipulate the Electrocatalytic Pathway for Zn‐Air Battery and Water Splitting

• Published in: Advanced energy materials 2023-01, Vol.13 (3), p.n/a
• Main Authors: Yang, Anzhou, Su, Keying, Lei, Wu, Tang, Yawen, Qiu, Xiaoyu
• Format: Article
• Language: English
• Subjects: Catalysts; Catalytic activity; electronic reciprocity; Hydrogen evolution; Metal air batteries; Obstructions; Reciprocity; Recyclability; single atomic sites; ternary metals; Water splitting; water splitting devices; Work breaks; Zinc-oxygen batteries; zinc‐air batteries
• ISSN: 1614-6832; 1614-6840
• DOI: 10.1002/aenm.202203150

Ternary metal catalysts hold great promise in complementary functionality and synergistic interplay, which are promising for combined reactions involving multi‐intermediates. However, simultaneously downscaling all three metal species into single‐atom level still remains challenge. Herein, a universal metal encapsulation‐segregation‐overlay strategy is designed to realize the fabrication of heterogeneous M1N4‐C‐M2N4‐C‐M3N4 ternary single‐atoms (TSAs)‐based catalysts, with well‐defined configuration and threefold enhancement of single‐atom loading (IrPtCu TSAs, up to 21.24 wt%). Taking non‐precious‐metallic CoN4‐C‐NiN4‐C‐FeN4 TSAs for instance, the integration of triple‐decker single‐atoms affords strong electronic reciprocity, with interbedded Ni donating electrons for both Fe and Co, thereby simultaneously enhancing the catalytic activity for oxygen reduction, oxygen evolution, and hydrogen evolution through a “site‐selective master‐servant” mechanism. Thanks to the mutually assisted tri‐functionality, the CoN4‐C‐NiN4‐C‐FeN4 TSAs‐electrode takes on alternatating master/servant roles to enable outstanding recyclability for energy devices. This work breaks the obstructions in synthesis and fundamental study of TSAs, providing insights into atomic material design for complicated catalytic reactions. This work reports a universal strategy to fabricate heterogeneous ternary metal single atoms‐based catalysts. With threefold enhancement of metal loading and strong electronic reciprocity, CoN4‐C‐NiN4‐C‐FeN4 affords a “site‐selective master‐servant” mechanism to enhance the catalytic activity of oxygen reduction, oxygen evolution, and hydrogen evolution for zinc‐air batteries and water splitting.