Solid-state stepwise temperature-programmable synthesis of bioinspired Fe-N-C oxygen reduction electrocatalyst featuring Fe-N_(5)configuration  

作　　者：Wei Sang Somboon Chaemchuen Longyang Zhang Zechen Wang Xingchuan Li Cocoro Andrew Nagasaka Mo Xiong Naoki Ogiwara Cheng Chen Zhao Wang Jian Zhang Francis Verpoort Shichun Mu Zongkui Kou Tingting Wang 

机构地区：[1]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China [2]Department of Basic Science,School of Arts and Sciences,The University of Tokyo,Komaba,Meguro-ku,Tokyo 153-8902,Japan [3]MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter,School of Physics,Xi’an Jiao tong University,Xi’an 710049,China [4]Sanya Science and Education Innovation Park of Wuhan University of Technology,Sanya 572000,China [5]Department of Chemical Engineering,Faculty of Engineering,Mahidol University,Nakhon Pathom 73170,Thailand [6]School of Mathematical&Physical Sciences,Wuhan Textile University,Wuhan 430200,China [7]Joint Institute of Chemical Research(FFMiEN),Peoples Friendship University of Russia(RUDN University),6 Miklukho-Maklaya Str.,117198 Moscow,Russia [8]National Research Tomsk Polytechnic University,Lenin Avenue 30,634050 Tomsk,Russia [9]Hubei Key Laboratory of Ferro,&Piezo-electric Materials and Devices,Faculty of Physics and Electronic Sciences,Hubei University,Wuhan 430062,China [10]School of Chemistry and Chemical Engineering,Hainan University,Haikou 57022,China

出　　处：《Nano Research》2025年第3期654-665,共12页纳米研究(英文版)

基　　金：financial support of the Fundamental Research Funds for the Central Universities(No.40120631);the National Natural Science Foundation of China(No.52202291).

摘　　要：The bioinspired Fe-N-C features an asymmetric Fe-N_(5)configuration to produce active metal-oxygen intermediates by introducing axial N ligand into a symmetric Fe-N_(4) structure,enabling highly active oxygen reduction reaction(ORR).However,the artificial creation of active Fe-N_(5)configuration with a direct,facile and green method has been rarely developed yet,as current techniques involve complex processes and costly precursors.Herein,we advance a novel solid-state stepwise temperature-programmable(SST)route to directly produce bioinspired Fe-N_(5)-C.We then demonstrate that such a Fe-N_(5)-C exhibits a quite higher half-wave potential(0.92 V)with 22-fold faster ORR kinetics(15.6 mA·cm^(−2)@0.85 V)over that of the commercial Pt/C counterpart.Indeed,we perform density functional theory(DFT)to find that the Fe is discharged with an extra 0.1 e^(−)through the axially coordinate N ligand,which significantly enhances the ability to activate O_(2) and enables an easier desorption of the crucial intermediate ^(*)OH on the Fe-N_(5)configuration over the conventional Fe-N_(4) structure.

关 键 词：single atom catalysts Fe-N_(5)coordination solvent-free synthesis oxygen reduction reaction(ORR) metal-air battery 

分 类 号：O62[理学—有机化学]