Tuning the charge distribution and crystal field of iron single atoms via iron oxide integration for enhanced oxygen reduction reaction in zinc-air batteries  

作　　者：Feifei Zhang Yinlong Zhu Yijun Zhong Jing Zou Yu Chen Lianhai Zu Zhouyou Wang Jack Jon Hinsch Yun Wang Lian Zhang Zongping Shao Huanting Wang 

机构地区：[1]Department of Chemical and Biological Engineering,Monash University,Clayton,VIC 3800,Australia [2]Institute for Frontier Science,Nanjing University of Aeronautics and Astronautics,Nanjing 210016,Jiangsu,China [3]WA School of Mines:Minerals,Energy and Chemical Engineering(WASM-MECE),Curtin University,Perth,WA 6102,Australia [4]Key Laboratory of Interfacial Physics and Technology,Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201800,China [5]Monash Centre for Electron Microscopy,Monash University,Clayton,VIC 3800,Australia [6]Department of Chemical Engineering,The University of Melbourne,Parkville,VIC 3010,Australia [7]Centre for Catalysis and Clean Energy,School of Environment and Science,Griffith University,Gold Coast Campus,Southport,QLD 4222,Australia

出　　处：《Journal of Energy Chemistry》2023年第10期154-163,I0006,共11页能源化学（英文版）

基　　金：supported by the Australian Research Council Australian Laureate Fellowship(No.FL200100049);the support of Natural Science Foundation for Young Scholars of Jiangsu Province(No.BK20220879);National Natural Science Foundation for Young Scholars of China(No.22209072);Monash University for a PhD scholarship as part of the university support for establishment of the ARC Research Hub for Energy-efficient Separation(H170100009)。

摘　　要：Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts.

关 键 词：Single-atom catalysts Oxide nanoclusters Electronic interactions Oxygen reduction reaction Zn-air battery 

分 类 号：O643.36[理学—物理化学] TM911.41[理学—化学]