Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction

doi:10.1007/s40242-020-0101-7

高等学校化学研究 ›› 2020, Vol. 36 ›› Issue (3): 453-458.doi: 10.1007/s40242-020-0101-7

Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction

WANG Yuqing¹, TAO Li¹, CHEN Ru¹, LI Hao¹, SU Hui², ZHANG Nana¹, LIU Qinghua², WANG Shuangyin¹

1. State Key Laboratory of Chemo/Bio-sensing and Chemometrics, Provincial Hunan Key Laboratory for Graphene Materials and Devices, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, P. R. China;
2. USA National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China

收稿日期:2020-04-10 修回日期:2020-04-27 出版日期:2020-06-01 发布日期:2020-04-27
通讯作者: CHEN Ru, WANG Shuangyin E-mail:chenru@hnu.edu.cn;shuangyinwang@hnu.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China(Nos.21701043, 21573066, 21825201), the Provincial Natural Science Foundation of Hunan, China(Nos.2016JJ1006, 2016TP1009), the Hunan Provincial Innovation Foundation for Postgraduate, China(No.CX2018B182) and the Open Project Program of Key Laboratory of Low Dimensional Materials & Application Technology(Xiangtan University), Ministry of Education, China(No.KF20180202).

Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction

WANG Yuqing¹, TAO Li¹, CHEN Ru¹, LI Hao¹, SU Hui², ZHANG Nana¹, LIU Qinghua², WANG Shuangyin¹

1. State Key Laboratory of Chemo/Bio-sensing and Chemometrics, Provincial Hunan Key Laboratory for Graphene Materials and Devices, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, P. R. China;
2. USA National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China

Received:2020-04-10 Revised:2020-04-27 Online:2020-06-01 Published:2020-04-27
Contact: CHEN Ru, WANG Shuangyin E-mail:chenru@hnu.edu.cn;shuangyinwang@hnu.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China(Nos.21701043, 21573066, 21825201), the Provincial Natural Science Foundation of Hunan, China(Nos.2016JJ1006, 2016TP1009), the Hunan Provincial Innovation Foundation for Postgraduate, China(No.CX2018B182) and the Open Project Program of Key Laboratory of Low Dimensional Materials & Application Technology(Xiangtan University), Ministry of Education, China(No.KF20180202).

摘要/Abstract

摘要： Exploring cost-effective and high-performance oxygen reduction reaction(ORR) electrocatalysts to replace precious platinum-based materials is crucial for developing electrochemical energy conversion devices but remains a great challenge. Herein, Fe single atoms anchored on nanosheet-linked, defect-rich, highly N-doped 3D porous carbon(Fe-SAs/NLPC) electrocatalysts were obtained by pyrolyzing salt-sealed Fe-doped zeolitic imidazolate frameworks(ZIFs). NaCl functions both as pore-forming agent and closed nanoreactor, which can not only lead to the formation of defects-rich three-dimensional interconnected structures with high N-doping content to expose abundant active sites, promote mass transfer and electron transfer, but also facilitate the effective incorporation of Fe to form Fe-N_x active sites without aggregation. These unique characteristics render Fe-SAs/NLPC outstanding electrocatalytic activity for ORR, with one-set potential of 0.96 V and high kinetic current density(j_K) of 33.32 mA/cm² in alkaline medium, which surpass the values of most nonprecious-metal catalysts and even commercial Pt/C.

关键词: Single-atom catalyst, Porous carbon, Non-precious metal, Oxygen reduction reaction

Abstract: Exploring cost-effective and high-performance oxygen reduction reaction(ORR) electrocatalysts to replace precious platinum-based materials is crucial for developing electrochemical energy conversion devices but remains a great challenge. Herein, Fe single atoms anchored on nanosheet-linked, defect-rich, highly N-doped 3D porous carbon(Fe-SAs/NLPC) electrocatalysts were obtained by pyrolyzing salt-sealed Fe-doped zeolitic imidazolate frameworks(ZIFs). NaCl functions both as pore-forming agent and closed nanoreactor, which can not only lead to the formation of defects-rich three-dimensional interconnected structures with high N-doping content to expose abundant active sites, promote mass transfer and electron transfer, but also facilitate the effective incorporation of Fe to form Fe-N_x active sites without aggregation. These unique characteristics render Fe-SAs/NLPC outstanding electrocatalytic activity for ORR, with one-set potential of 0.96 V and high kinetic current density(j_K) of 33.32 mA/cm² in alkaline medium, which surpass the values of most nonprecious-metal catalysts and even commercial Pt/C.

Key words: Single-atom catalyst, Porous carbon, Non-precious metal, Oxygen reduction reaction

WANG Yuqing, TAO Li, CHEN Ru, LI Hao, SU Hui, ZHANG Nana, LIU Qinghua, WANG Shuangyin. Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction[J]. 高等学校化学研究, 2020, 36(3): 453-458.

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Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction

Atomically Dispersed Fe on Nanosheet-linked, Defect-rich, Highly N-Doped 3D Porous Carbon for Efficient Oxygen Reduction

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