Cubic hollow porous carbon with defective-edge Fe-N4 single-atom sites for high-performance Zn-air batteries

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

doi:10.1016/j.jmst.2023.09.025

Cubic hollow porous carbon with defective-edge Fe-N₄ single-atom sites for high-performance Zn-air batteries

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

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

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-N₄ 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.

Original language	English
Pages (from-to)	82-90
Number of pages	9
Journal	Journal of Materials Science and Technology
Volume	181
DOIs	https://doi.org/10.1016/j.jmst.2023.09.025
State	Published - 10 May 2024
Externally published	Yes

Keywords

DFT calculations
Defective-edge Fe-N sites
Hollow porous catalyst
ORR
Zn-air battery

ASJC Scopus subject areas

Ceramics and Composites
Mechanics of Materials
Mechanical Engineering
Polymers and Plastics
Metals and Alloys
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.jmst.2023.09.025

Cite this

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title = "Cubic hollow porous carbon with defective-edge Fe-N4 single-atom sites for high-performance Zn-air batteries",

abstract = "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-N4 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 gZn−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.",

keywords = "DFT calculations, Defective-edge Fe-N sites, Hollow porous catalyst, ORR, Zn-air battery",

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

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year = "2024",

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doi = "10.1016/j.jmst.2023.09.025",

language = "English",

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TY - JOUR

T1 - Cubic hollow porous carbon with defective-edge Fe-N4 single-atom sites for high-performance Zn-air batteries

AU - Zhou, Shilong

AU - Chen, Chao

AU - Xia, Jiawei

AU - Li, Le

AU - Qian, Xingyue

AU - Yin, Fengxiang

AU - Dai, Guohong

AU - He, Guangyu

AU - Chen, Qun

AU - Chen, Haiqun

PY - 2024/5/10

Y1 - 2024/5/10

N2 - 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-N4 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 gZn−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.

AB - 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-N4 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 gZn−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.

KW - DFT calculations

KW - Defective-edge Fe-N sites

KW - Hollow porous catalyst

KW - ORR

KW - Zn-air battery

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