Single-atomic iron synergistic atom-cluster induce remote enhancement toward oxygen reduction reaction  

作　　者：Yayin Li Haomin Jiang Liu Lin Zemin Sun Genban Sun 

机构地区：[1]Beijing Key Laboratory of Energy Conversion and Storage Materials Institution,College of Chemistry,Beijing Normal University,Beijing 100875,China [2]Center for Advanced Materals Research College of Arts and Sciences,Experiment and Practice Innovation Education Center,Bejing Nomal University,Zhuhai 59 Guangdong,China

出　　处：《Journal of Energy Chemistry》2025年第3期413-420,共8页能源化学(英文版)

基　　金：supported by the National Natural Science Foundations of China(Nos:22271018,22309012 and 22302013);the NSF of Guangdong Province(Nos:2023A1515010554 and 2024A1515010307)。

摘　　要：The oxygen reduction reaction(ORR)could be effectively regulated by adjusting electron configurations and optimizing chemical bonds.Herein,we have achieved the modulation of electron distribution in Fe single atomic(Fe_(SA))sites through Fe atomic clusters(Fe_(AC))via a confined pyrolysis approach,thereby enhancing their intrinsic ORR activity.X-ray absorption spectroscopy has confirmed that the presence of iron atomic dusters could influence the electron distribution at Fe-N_(4)sites.The Fe_(SA)/Fe_(AC)-NC catalyst exhibits a half-wave potential of 0.88 V,surpassing the individual Fe_(SA)-NC structure.Through electronic structure analysis,it could be seen that iron atom clusters can affect Fe-N_(4)sites through long-range effects,and then effectively lower reaction barriers and enhance the reaction kinetics at Fe-N_(4)sites.The synthetic approach might pave the way for constructing highly active catalysts with tunable atomic structures,representing an effective and universal technique for electron modulation in M-N-C systems.This work provides enlightenment for the exploration of more efficient single-atom electrocatalysts and the optimization of the performance of atomic electrocatalysts.Furthermore,a zinc-air battery assembled using it on their cathode deliver a high peak power density(205.7 mW cm^(-2))and a high-specific capacity of 807.5 mA h g^(-1).This study offers a fresh approach to effectively enhance the synergistic interaction of between Fe single atom and Fe atomic clusters for improving ORR activity and energy storage.

关 键 词：Single atomic catalysts Atom-cluster induce effect Oxygen reduction reaction Fe-N4 sites 

分 类 号：O643.36[理学—物理化学]