Highly Reversible Anode-Free Lithium Metal Batteries Enabled by Porous Organic Cages with Subnano Lithiophilic Triangular Windows
Jipeng Xu, Kai Qu, Xinrui Li, Yan Cui, Jingkun Li, Honglai Liu, Cheng Lian
Abstract
The widespread application of anode-free lithium metal batteries (AFLMBs) is hindered by the severe dendrite growth and side reactions due to the poor reversibility of Li plating/stripping. Herein, our study introduces an ultrathin interphase layer of covalent cage 3 (CC3) for highly reversible AFLMBs. The subnano triangular windows in CC3 serve as a Li + sieve to accelerate Li + desolvation and transport kinetics, inhibit electrolyte decomposition, and form LiF- and Li 3 N-rich solid-electrolyte interphases. Moreover, the lithiophilic backbone of CC3 homogenizes Li + distribution and deposition with mitigated dendrite growth. Thus, CC3 promotes Li plating/stripping kinetics and reversibility, achieving an ultralong stability over 8000 h of the Cu@CC3 electrode. Furthermore, practical Cu@CC3/LiFePO 4 AFLMBs deliver a capacity retention (66%) over 600 cycles. This work emphasizes the effectiveness of CC3 to regulate the Li plating/stripping behavior, demonstrating the application potential of porous organic cages for enhancing the cycle life of AFLMBs.