Xu Jipeng, Qu Kai, Li Xinrui, Cui Yan, Li Jingkun, Liu Honglai, Lian Cheng
Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou 215123, China.
ACS Nano. 2025 Jan 21;19(2):2936-2943. doi: 10.1021/acsnano.4c16906. Epub 2025 Jan 8.
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 LiN-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 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.
无阳极锂金属电池（AFLMBs）的广泛应用受到锂电镀/剥离可逆性差导致的严重枝晶生长和副反应的阻碍。在此，我们的研究引入了一种用于高可逆AFLMBs的超薄共价笼3（CC3）界面层。CC3中的亚纳米三角形窗口用作锂筛，以加速锂去溶剂化和传输动力学，抑制电解质分解，并形成富含LiF和LiN的固体电解质界面。此外，CC3的亲锂主链使锂分布和沉积均匀化，减轻枝晶生长。因此，CC3促进了锂电镀/剥离动力学和可逆性，在Cu@CC3电极上实现了超过8000小时的超长稳定性。此外，实用的Cu@CC3/LiFePO AFLMBs在600次循环中容量保持率为66%。这项工作强调了CC3调节锂电镀/剥离行为的有效性，展示了多孔有机笼在延长AFLMBs循环寿命方面的应用潜力。
