期刊
NANO RESEARCH
卷 15, 期 9, 页码 8056-8064出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4424-1
关键词
N-doped hierarchical porous carbon/rGO composite; single-atom electrocatalyst; five N-coordinated Fe (Fe-N-5) single-atom sites; zinc-air battery; density functional theory (DFT) study
类别
资金
- National Natural Science Foundation of China [22078028, 22078027, 21978026]
A single-atom catalyst Fe-N-C/rGO SAC is prepared by pyrolyzing ZIF-8 and GO composite, which effectively promotes the oxygen reduction and oxygen evolution reactions for both liquid and solid-state ZABs, exhibiting excellent performance and reliable cycling stability.
Developing innovative and efficient non-precious-metal-group (non-PMG) electrocatalysts is crucial for the wide use of zinc-air batteries (ZABs). Herein, a single-atom catalyst (termed as Fe-N-C/rGO SAC) with unique five N-coordinated Fe (Fe-N-5) centers is prepared by pyrolyzing the composite of zeolitic-imidazolate-frameworks-8 (ZIF-8) and graphene oxide (GO). Specifically, the individual Fe site is stabilized by four equatorial and one axial N atoms donated by the N-doped carbon matrix and imidazole ring, respectively, thus forming an asymmetric electron depletion zone over the metal center, which can effectively promote the generation of reactive intermediates and accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) processes for ZABs. The rechargeable liquid ZAB with Fe-N-C/rGO catalyst exhibits an extremely high energy density (928.25 VVh.kg(-1)), a remarkable peak power density (107.12 mW.cm(-2)), and a long cycle life (400 h). Additionally, the corresponding flexible solid-state ZAB displays superior foldability and remarkable cycling stability. This work provides both experimental and theoretical guidance for rational design of non-PMG electrocatalyst-driven ZABs.
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