A self-regulated gradient interphase for dendrite-free solid-state Li batteries

Tengrui Wang; Jian Duan; Bao Zhang; Wei Luo; Xiao Ji; Henghui Xu; Ying Huang; Liqiang Huang; Zhenyou Song; Jiayun Wen; Chunsheng Wang; Yunhui Huang; John B. Goodenough

doi:10.1039/D1EE03604A

A self-regulated gradient interphase for dendrite-free solid-state Li batteries†

Tengrui Wang,‡^a Jian Duan,‡^a Bao Zhang,‡^b Wei Luo,

*^a Xiao Ji,^b Henghui Xu,^cd Ying Huang,^a Liqiang Huang,^a Zhenyou Song,^a Jiayun Wen,^a Chunsheng Wang,

*^b Yunhui Huang

*^d and John B. Goodenough

*^c

Author affiliations

* Corresponding authors

^a Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai 201804, China
E-mail: weiluo@tongji.edu.cn

^b Department of Chemical & Biomolecular Engineering, University of Maryland College Park, College Park, Maryland, USA
E-mail: cswang@umd.edu

^c Materials Science and Engineering Program and Department of Mechanical Engineering, The University of Texas at Austin, Austin 78712 TX, USA
E-mail: jgoodenough@mail.utexas.edu

^d State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
E-mail: huangyh@hust.edu.cn

Abstract

Solid-state Li metal batteries (SSLMBs) have emerged as an important energy storage technology that offers the possibility of both high energy density and safety by combining a Li metal anode (LMA), a high-capacity cathode and a nonflammable solid-state electrolyte (SSE). However, the major challenges of poor LMA/SSE interface wetting and the easy growth of Li dendrites in SSEs remain unsolved. Here, we have addressed these challenges by using a functional gradient Li anode (FGLA), which is formed through a self-regulated reaction between molten Li and AlF₃. A composition gradient of Li–LiAl–LiF is spontaneously formed from the reaction of molten Li with AlF₃ due to the large difference in interfacial energy between Li/LiAl and Li/LiF, where the LiAl reduces the interface resistance and LiF suppresses Li dendrites. The FGLA not only dramatically reduces the resistance at the FGLA/Li_6.5La₃Zr_1.5Ta_0.5O₁₂ (LLZTO) garnet SSE interface to ∼1 Ω cm⁻², but also largely increases the critical current density (CCD) to over 3.0 mA cm⁻² at room temperature. Moreover, the full cells paired with LiNi_0.5Co_0.2Mn_0.3O₂, sulfur and thick LiFePO₄ cathodes (∼2.8 mA h cm⁻²) also show excellent cycling performances. The FGLA design provides a great opportunity for safe and high-energy SSLMBs.

Energy & Environmental Science

A self-regulated gradient interphase for dendrite-free solid-state Li batteries†

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A self-regulated gradient interphase for dendrite-free solid-state Li batteries

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