Boosted electron accumulation around Fe atom by asymmetry coordinated FeN3S1 for efficient oxygen reduction reaction

Catalysts with atomically dispersed Fe–N4 active sites have emerged as promising alternatives for noble-metal catalysts in oxygen reduction reaction (ORR). However, the sluggish reaction kinetics limit their further utilization. Herein, asymmetry active sites FeN3S1 located on mesoporous carbon matr...

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Bibliographic Details
Published in:	International journal of hydrogen energy Vol. 90; pp. 1003 - 1011
Main Authors:	Liu, Chenhong, Yang, Xiaoli, Jia, Zhichao, Pan, Jialiang, Zhao, Fei, Ban, Yonghui, Cui, Xiumei, Bai, Zhengyu, Yang, Lin
Format:	Journal Article
Language:	English
Published:	Elsevier Ltd 11-11-2024
Subjects:	Asymmetric coordination Mesoporous structure Optimizing adsorption energy Oxygen reduction reaction Zn-air battery Zn-air battery Asymmetric coordination Mesoporous structure Oxygen reduction reaction Optimizing adsorption energy
Online Access:	Get full text
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Summary:	Catalysts with atomically dispersed Fe–N4 active sites have emerged as promising alternatives for noble-metal catalysts in oxygen reduction reaction (ORR). However, the sluggish reaction kinetics limit their further utilization. Herein, asymmetry active sites FeN3S1 located on mesoporous carbon matrix (Fe–N3S1/Cmeso) are constructed and verified as efficient ORR catalysts with fast reaction kinetics. The synthesized Fe–N3S1/Cmeso catalysts exhibit a half-wave potential of 0.92 V in alkaline electrolyte, a higher power density (178 mW cm−2) and a long-term durability (350 h) in Zn-Air battery. Mechanism study demonstrates that the specific structure induces accumulated electronic density and decreased d band center of Fe atoms which optimize the adsorption energy with OH∗ intermediates thus boosting the intrinsic activity. Moreover, the uniform mesoporous structure significantly increases the accessibility of active sites. This work offers a new perspective to optimize the adsorption strength of reaction intermediates for enhanced ORR. [Display omitted] •Asymmetry active sites of Fe–N3S1 located on mesoporous substrate were constructed.•The adsorption energy of oxygenated intermediates was optimized.•Mesoporous substrate possesses highly exposed sites and fast mass transportation.•Fe–N3S1/Cmeso catalysts exhibit superior ORR performance and long-term durability.
ISSN:	0360-3199
DOI:	10.1016/j.ijhydene.2024.10.049