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Start Over Author "He, Guangyu" Publisher elsevier b.v.
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50. Cubic hollow porous carbon with defective-edge Fe-N4 single-atom sites for high-performance Zn-air batteries.

Author

Zhou, Shilong, Chen, Chao, Xia, Jiawei, Li, Le, Qian, Xingyue, Yin, Fengxiang, Dai, Guohong, He, Guangyu, Chen, Qun, and Chen, Haiqun

Subjects
LITHIUM cells, OPEN-circuit voltage, DENSITY functional theory, ALKALINE batteries, ELECTRONIC structure, MASS transfer, OXYGEN reduction, POLYMERS
Abstract

• Unique defective-edge Fe-N 4 moieties with optimized intrinsic activity were constructed. • The cubic hollow hierarchical porous structure endows abundant active sites and faster ions/mass transfer. • The catalyst exhibits superior ORR and OER activity to that of commercial Pt/C-RuO 2. • The homemade liquid and flexible solid-state ZABs exhibit a promising prospect for practical application. Regulating the local coordination of Fe active center can further improve the oxygen reduction reaction (ORR) performance of Fe-N-C catalyst to meet the practical application requirements of zinc-air batteries (ZABs). Herein, carbon vacancies modified hollow porous catalysts (C-FeZ8@PDA-950) are constructed by microenvironment modulation, achieving the efficient utilization of active sites and optimization of electronic structure. Density functional theory (DFT) calculations confirm that the defective-edge Fe-N 4 sites can weaken the adsorption free energy of OH*, and hinder the dissolution of Fe center, significantly accelerating the ORR process for ZABs. The rechargeable liquid ZABs equipped with C-FeZ8@PDA-950 display high specific capacity (819.95 mAh g Zn −1) and excellent long-cycling life (over 500 h). Furthermore, the relevant flexible all-solid-state ZABs also display outstanding folding performance under various bending angles. This work will provide insights into optimizing the electronic structure to improve electrocatalytic performance in the energy conversion and storage area. A hollow hierarchical porous C-FeZ8@PDA-950 catalyst with atomic defectiveedge Fe-N4 moieties modified by carbon vacancies is constructed via a combined approach following the order of electrostatic absorption, polymer coating, and pyrolysis, showing superior ORR and OER activity. The homemade liquid and flexible solid-state zinc-air batteries demonstrate excellent performance in terms of open-circuit voltage, discharging specific capacity, and long-term durability. [Display omitted] [ABSTRACT FROM AUTHOR]

Published
2024
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