Li + Ion-Dipole Interaction-Enabled a Dynamic Supramolecular Elastomer Interface Layer for Dendrite-Free Lithium Metal Anodes

作者：Jing Chen, Xuetian Deng, Xin Jia, Yang Gao, Han Chen, Zhiqun Lin, Shujiang Ding · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c08766 · 被引用次数：60 · 研究领域：Advanced Battery Materials and Technologies、Conducting polymers and applications、Advancements in Battery Materials

The unstable lithium (Li)/electrolyte interface, causing inferior cycling efficiency and unrestrained dendrite growth, has severely hampered the practical deployment of Li metal batteries (LMBs), particularly in carbonate electrolytes. Herein, we present a robust approach capitalizing on a dynamic supramolecular elastomer (DSE) interface layer, which is capable of being reduced with Li metal to spontaneously form strong Li + ion-dipole interaction, thereby enhancing interfacial stability in carbonate electrolytes. The soft phase in the DSE structure enables fast Li + transport via loosely coordinated Li + –O interaction, while the hard phase, rich in electronegative lithiophilic sites, drives the generation of fast-ion-conducting solid electrolyte interface components, including Li 3 N and Li 2 S. Furthermore, the dynamically resilient DSE network composed of soft and hard phases protects Li anodes from electrolyte corrosion and accommodates volume changes during cycling. All features of the DSE layer synergistically facilitate uniform Li + deposition and suppress Li dendrite propagation, ensuring a stable and dendrite-free Li anode. Consequently, the symmetric Li||Li cell incorporating the DSE layer achieves cycling stability exceeding 6000 h under 1 mA cm –2 and 1 mA h cm –2 conditions. Furthermore, full cell pairing DSE/Li anode with LiFePO 4 (LFP) or high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes exhibits high-efficiency Li deposition and cycling stability, eve...