中国科学技术大学王献红研究小组揭示了可逆锂盐催化制备闭环可回收固态聚合物电解质。这一研究成果于2025年2月24日发表在国际顶尖学术期刊《美国化学会杂志》上。

研究组提出了一种创新的固体聚合物电解质（spe）闭环设计，通过双（三氟甲烷）磺酰亚胺锂（LiTFSI）的可逆催化实现聚合和解聚。TFSI-和醇之间氢键加合物的形成引发了Li⁺活化的碳酸三亚甲基（TMC）的原位开环聚合，生成了定义明确的SPE。经过精细的结构优化，SPE在室温下的离子电导率为1.62×10^-3 S cm^-1，高压稳定性高达4.7V。组装的Li||NCM811具有良好的循环稳定性，在100次循环中保持88%的容量。在使用寿命结束时，LiTFSI可以在180°C下促进聚碳酸酯基SPE的选择性解聚，而无需引入外部催化剂，回收TMC单体（>90%）和LiTFSI （>98%）进行再聚合。这项工作突出了闭环可回收SPE的重大进步，也是朝着可持续锂电池技术迈出的重要一步。

据悉，锂电池生产和处置的快速扩张带来了相当大的可持续性挑战，强调了对回收的迫切需求。然而，目前的方法主要集中在阴极上的金属，而电解质很少被回收利用。

附：英文原文

Title: Closed-Loop Recyclable Solid-State Polymer Electrolytes Enabled by Reversible Lithium Salt Catalysis

Author: Pei Chen, Shunjie Liu, Hao Zhou, Shuo Yan, Dongxuan Zhang, Xuan Pang, Xuesi Chen, Xianhong Wang

Issue&Volume: February 24, 2025

Abstract: The rapid expansion in lithium battery production and disposal presents considerable sustainability challenges, emphasizing the critical need for recycling. However, current methods predominantly focus on metals from cathodes, while electrolytes have rarely been recycled. Here, we propose an innovative closed-loop design for solid polymer electrolytes (SPEs), enabled by reversible catalysis of lithium bis(trifluoromethane) sulfonimide (LiTFSI) in both polymerization and depolymerization. The formation of a hydrogen-bonded adduct between TFSI– and alcohol initiates the in situ ring-opening polymerization of Li⁺-activated trimethylene carbonate (TMC), generating well-defined SPEs. With delicate structural optimization, the SPE achieves an outstanding ionic conductivity of 1.62 × 10^–3 S cm^–1 at room temperature with robust high-voltage stability up to 4.7 V. The assembled Li||NCM811 demonstrates promising cycling stability with 88% capacity retention over 100 cycles. Upon end-of-life, LiTFSI facilitates selective depolymerization of the polycarbonate-based SPE at 180 °C without introducing external catalysts, recovering both TMC monomer (>90%) and LiTFSI (>98%) for reuse. This work highlights a significant advance in closed-loop recyclable SPEs and a vital step toward sustainable lithium battery technology.

DOI: 10.1021/jacs.4c17035

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c17035