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Research Article

Probing the active sites of 2D nanosheets with Fe-N-C carbon shell encapsulated FexC/Fe species for boosting sodium-ion storage performances

Huicong Xia1,2, Pengfei Yuan3, Lingxing Zan2,5, Gan Qu1, Yunchuan Tu2, Kaixin Zhu2, Yifan Wei1, Zeyu Wei2, Fangying Zheng2, Mo Zhang2,4, Yongfeng Hu6, Dehui Deng2( ), Jianan Zhang1( )
College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
State Key Laboratory of Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
College of Physics and Engineering, Zhengzhou University, Zhengzhou 450001, China
College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
Key Laboratory of Chemical Reaction Engineering of Shaanxi Province, College of Chemistry & Chemical Engineering, Yan’an University, Yan’an 716000, China
Canadian Light Source, 44 Innovation Boulevard Saskatoon, Saskatoon S7N 2V3, Canada
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Graphical Abstract

Fe-N-C graphitic carbon layers-encapsulating Fe3C species within hard carbon nanosheets (Fe-N-C/Fe3C@HCNs) were rationally engineered by pyrolysis of self-assembled polymer. The coupling effect of atomically dispersed Fe-N-C and Fe3C species play a significant role in enhancing the binding ability towards Na+ ions, allowing the robust rate performance and prolonged cycling life for sodium-ion battery.

Abstract

Developing stable but high active metal-nitrogen-carbon (M-N-C)-based hard carbon anode is a promising way to be the alternatives to graphene and blank hard carbon for sodium-ion batteries (SIBs), requiring the precise tailoring of the electronic structure for optimizing the Na+ intercalation behavior, yet is greatly challenging. Herein, Fe-N-C graphitic layer-encapsulating Fe3C species within hard carbon nanosheets (Fe-N-C/Fe3C@HCNs) are rationally engineered by pyrolysis of self-assembled polymer. Impressively, the Fe-N-C/Fe3C@HCNs exhibit outstanding rate capacity (242 mAh·g−1 at 2,000 mA·g−1), which is 2.1 and 4.2 times higher than that of Fe-N-C and N-doped carbon (N-C), respectively, and prolonged cycling stability (176 mAh·g−1 at 2,000 mA·g−1 after 2,000 cycles). Theoretical calculations unveil that the Fe3C species enhance the electronic transfer from Na to Fe-N-C, resulting in the charge redistribution between the interfaces of Fe3C and Fe-N-C. Thus, the optimized adsorption behavior towards Na+ reduces the thermodynamic energy barriers. The synergistic effect of Fe3C and Fe-N-C species maintains the structural integrity of electrode materials during the sodiation/desodiation process. The in-depth insight into the advanced Na+ storage mechanisms of Fe3C@Fe-N-C offers precise guidance for the rational establishment of confinement heterostructures in SIBs.

Keywords

Fe-N-C/Fe3C species encapsulatedcarbon nanosheetssodium-ion storagedensity functional theory

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Nano Research
Volume 15 Issue 8,
August 2022
Pages 7154-7162
DOI: 10.1007/s12274-021-3992-9
Cite this article:
Xia H, Yuan P, Zan L, et al. Probing the active sites of 2D nanosheets with Fe-N-C carbon shell encapsulated FexC/Fe species for boosting sodium-ion storage performances. Nano Research, 2022, 15(8): 7154-7162. https://doi.org/10.1007/s12274-021-3992-9
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Received: 20 September 2021
Revised: 20 October 2021
Accepted: 11 November 2021
Published: 15 December 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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