Alliance of atomic-scale/nanoscale Fe/Co active sites with hierarchically porous N-doped carbon frameworks for efficient electrocatalytic oxygen reduction  

作　　者：Hai-Hua Yang Xiao-Rong Qian Na Zhang Xia-Ting Jia Zhi-Yan Wen Xiao-Bo Chen Min-Jie Zhou 

机构地区：[1]Key Laboratory of Hunan Province for Advanced Carbon-Based Functional Materials,Hunan Institute of Science and Technology,Yueyang,414006,China [2]School of Chemistry and Chemical Engineering,Hunan Institute of Science and Technology,Yueyang,414006,China [3]School of Physics and Electronic Science,Hunan Institute of Science and Technology,Yueyang,414006,China [4]Department of Chemistry,University of Missouri-Kansas City,Kansas City,64111,USA

出　　处：《Rare Metals》2023年第11期3766-3779,共14页稀有金属（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (No.51972109);the Natural Science Foundation of Hunan Province (No.2023JJ30276);the Scientific Research Fund of Hunan Provincial EducationDepartment,China (Nos.22A0473 and 20A225);the Postgraduate Research Innovation Fund of Hunan Institute of Science and Technology (No.2022-38)。

摘　　要：Ingenious establishment of transition metal-nitrogen-carbon electrocatalysts with diverse catalytic active sites and hierarchically porous frameworks is highly significant to boost the oxygen reduction reaction(ORR)in Zn-air batteries(ZABs).In this study,Fe/Co co-doped zeolitic imidazolium frameworks(ZIFs)and graphitic carbon nitride(g-C_(3)N_(4))were integrated and pyrolyzed to construct carbon-based electrocatalysts containing Fe,Co and N elements(labelled as Co-CoFe@NRPC),in which atomic-sc ale FeN_x and CoN_x,and nano scale metallic Co and CoFe alloy moieties were aligned with hierarchically porous N-doped carbon frameworks constructed by interconnected micropolyhedrons,nano tubes and nanosheets.The diverse active moieties guaranteed excellent intrinsic catalytic activity,while the hierarchically porous N-doped carbon frameworks ensured admirable accessibility of the catalytic active sites,excellent electrical conductivity,satisfactory mass transport and good durability.Expectedly,the optimized Co-CoFe@NRPC-90(with 90 mg g-C_(3)N_(4) added)electrocatalyst exhibited excellent ORR performance with a high half-wave potential of 885 mV(vs.reversible hydrogen electrode(RHE)),diffusion-limiting current density of 6.15 mA·cm^(-2),desirable durability and methanol tolerance.Simultaneously,the liquid ZAB established with Co-CoFe@NRPC-90 as an air-cathode electrocatalyst manifested an outstanding power density(281 mW·cm^(-2))and specific capacity(820.9 mAh·g_(Zn)^(-1)),transcending the liquid ZAB based on a commercial Pt/C electrocatalyst.

关 键 词：Fe/Co co-doped zeolitic imidazolium frameworks Graphitic carbon nitride Transition metal-nitrogen-carbon electrocatalyst Oxygen reduction reaction(ORR) 

分 类 号：TM911.41[电气工程—电力电子与电力传动] O643.36[理学—物理化学]