Journal of Energy Chemistry ›› 2023, Vol. 76 ›› Issue (1): 648-656.DOI: 10.1016/j.jechem.2022.09.025

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In situ generation of Li3N concentration gradient in 3D carbon-based lithium anodes towards highly-stable lithium metal batteries

Wenzhu Caoa, Weimin Chena,*, Mi Lua, Cheng Zhanga, Du Tiana, Liang Wangb,*, Faquan Yua,*   

  1. aKey Laboratory for Green Chemical Process of Ministry of Education, Hubei Key Laboratory for Novel Reactor and Green Chemistry Technology, Hubei Engineering Research Center for Advanced Fine Chemicals, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, Hubei, China;
    bChongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences, Chongqing 400714, China
  • Received:2022-07-06 Revised:2022-09-11 Accepted:2022-09-13 Published:2023-01-10
  • Contact: *E-mail addresses: wmchen@wit.edu.cn (W. Chen), wangliang@cigit.ac.cn (L. Wang), fyu@wit.edu.cn (F. Yu).

Abstract: The uncontrolled dendrite growth of lithium metal anodes (LMAs) caused by unstable anode/electrolyte interface and uneven lithium deposition have impeded the practical applications of lithium metal batteries (LMBs). Constructing a robust artificial solid electrolyte interphase (SEI) and regulating the lithium deposition behavior is an effective strategy to address these issues. Herein, a three-dimensional (3D) lithium anode with gradient Li3N has been in-situ fabricated on carbon-based framework by thermal diffusion method (denoted as CC/Li/Li3N). Density functional theory (DFT) calculations reveal that Li3N can effectively promote the transport of Li+ due to the low energy barrier of Li+ diffusion. As expected, the Li3N-rich conformal artificial SEI film can not only effectively stabilize the interface and avoid parasitic reactions, but also facilitate fast Li+ transport across the SEI layer. The anode matrix with uniformly distributed Li3N can enable homogenous deposition of Li, thus preventing Li dendrite propagation. Benefiting from these merits, the CC/Li/Li3N anode achieves ultralong-term cycling for >1000 h at a current density of 2 mA cm-2 and dendrite-free Li deposition at an ultrahigh rate of 20 mA cm-2. Moreover, the full cells coupled with LiFePO4 cathodes show extraordinary cycling stability for >300 cycles in liquid-electrolyte-based batteries and display a high-capacity retention of 96.7% after 100 cycles in solid-state cells, demonstrating the promising prospects for the practical applications of LMBs.

Key words: Li3N, Gradient, Three-dimensional host, Interphase, Lithium metal anode