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29-09-2023 | Original Article

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

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

Published in: Rare Metals | Issue 11/2023

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Abstract

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-C₃N₄) were integrated and pyrolyzed to construct carbon-based electrocatalysts containing Fe, Co and N elements (labelled as Co–CoFe@NRPC), in which atomic-scale FeN_x and CoN_x, and nanoscale metallic Co and CoFe alloy moieties were aligned with hierarchically porous N-doped carbon frameworks constructed by interconnected micropolyhedrons, nanotubes 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-C₃N₄ 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.

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Title: Alliance of atomic-scale/nanoscale Fe/Co active sites with hierarchically porous N-doped carbon frameworks for efficient electrocatalytic oxygen reduction
Authors: Hai-Hua Yang
Xiao-Rong Qian
Na Zhang
Xia-Ting Jia
Zhi-Yan Wen
Xiao-Bo Chen
Min-Jie Zhou
Publication date: 29-09-2023
Publisher: Nonferrous Metals Society of China
Published in: Rare Metals / Issue 11/2023
Print ISSN: 1001-0521
Electronic ISSN: 1867-7185
DOI: https://doi.org/10.1007/s12598-023-02397-8

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