Rational Design of a Cross-Linked Composite Solid Electrolyte for Li-Metal Batteries

Changhao Tian; Mengyuan Song; Jiantao Tang; Haoyang Yuan; Chao Ai; Huajun Cao; Tao Huang; Aishui Yu

doi:10.1021/acsami.3c15456

Rational Design of a Cross-Linked Composite Solid Electrolyte for Li-Metal Batteries

ACS Appl Mater Interfaces. 2024 Jan 10;16(1):1535-1542. doi: 10.1021/acsami.3c15456. Epub 2023 Dec 22.

Authors

Changhao Tian¹, Mengyuan Song¹, Jiantao Tang¹, Haoyang Yuan¹, Chao Ai², Huajun Cao², Tao Huang³, Aishui Yu^{1

3}

Affiliations

¹ Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, China.
² Huawei Technologies Co., Ltd., Shenzhen 518116, China.
³ Laboratory of Advanced Materials, Fudan University, Shanghai 200438, China.

PMID: 38134330
DOI: 10.1021/acsami.3c15456

Abstract

The interfacial problem caused by solid-solid contact is an important issue faced by a solid-state electrolyte (SSE). Herein, a cross-linked composite solid electrolyte (CSE) poly(vinylene carbonate) (PVCA)─ethoxylated trimethylolpropane triacrylate (ETPTA)─Li_1.5Al_0.5Ge_1.5(PO₄)₃ (LAGP) (PEL) is prepared by in situ thermal polymerization. The ionic conductivity and Li⁺ transference number (t_Li⁺) of PEL increase significantly due to the addition of LAGP, which can reach 1.011 × 10^-4 S cm^-1 and 0.451 respectively. The electrochemical stable window is also widened to 4.68 V. Benefiting from the integrated interfacial structure, the assembled coin cell shows low interfacial resistance. The all-solid-state NCM622|PEL|Li coin cell exhibits an initial discharge capacity of 169.7 mA h g^-1 and 70% capacity retention over 100 cycles at 0.2 C, demonstrating excellent cycling stability.

Keywords: Li1.5Al0.5Ge1.5(PO4)3; composite solid electrolyte; in situ thermal polymerization; integrated structure; lithium-metal battery.