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Work-function effect of Ti3C2/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Abstract

In the quest to enhance the efficiency of sodium-ion batteries, the dynamics of solid electrolyte interphase (SEI) formation are of paramount importance. The SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the battery. Herein, a novel two-dimensional Ti3C2 fragments enmeshed on iron-nitrogen-carbon (Fe-N-C) nanosheets (Ti3C2/Fe-N-C) has been synthesized. This electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption, thus augmenting battery performance. Density functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti3C2/Fe-N-C interface is 0.81 eV, significantly lower than the Ti3C2 (1.23 eV). This process is driven by the electron transportation from Ti3C2 to Fe-N-C substrate, facilitated by their work-function difference, leading to the formation of ferromagnetic Fe species, which possesses Fe 3d \(\mathrm{d}_{xz}\mathrm{d}_{yz}\mathrm{d}_{z^{2}}\) orbitals and undergoes hybridization with the π and σ orbitals of NaF, creating a key intermediate during charging. This process diminishes the antibonding energy and attenuates the orbital interaction with NaF, thus reducing the activation energy and improving the SEI formation reaction kinetics. Consequently, it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

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Acknowledgement

This work was supported by the National Natural Science Foundation of China (Nos. U22A20107, 22162026, and 42050203), the Science and Technology Research and Develpoment Program Joint Fund Project of Henan Provincial (No. 222301420001), the Distinguished Young Scholars Innovation Team of Zhengzhou University (No. 32320275), Key Research Projects of University in Henan Province (No. 24A150041), Henan Province Science and Technology Research Projects (No. 242102240106), and Postdoctoral Fellowship Program of CPSF (No. GZC20232382). The authors also gratefully acknowledge the BL14W1 and BL11B at Shanghai Synchrotron Radiation Facilities (SSRF) and beamline 4B9A at Beijing Synchrotron Radiation Facility (BSRF) for the XAFS measurements.

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  1. Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Huicong Xia, Yifan Wei, Yue Yu & Jia-Nan Zhang

  2. Key Laboratory of Materials Physics of Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, 450001, China

    Chong-Xin Shan

  3. Key Laboratory of Chemical Reaction Engineering of Shaanxi Province, College of Chemistry and Chemical Engineering, Yan’an University, Yan’an, 716000, China

    Lingxing Zan

  4. Center for High Pressure Science and Technology Advanced Research, Pudong, Shanghai, 201203, China

    Hongliang Dong & Jinfu Shu

  5. Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, China

    Huicong Xia

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Xia, H., Zan, L., Dong, H. et al. Work-function effect of Ti3C2/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage. Nano Res. (2024). https://doi.org/10.1007/s12274-024-6693-3

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