Yang Wu, Tang Shijun, Yang Xuerui, Zheng Xuefan, Wu Yuqi, Zheng Chenxi, Chen Guiwei, Gong Zhengliang, Yang Yong
College of Energy, Xiamen University, Xiamen 361102, China.
State Key Laboratory for Physical Chemistry of Solid Surface, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
ACS Appl Mater Interfaces. 2022 Nov 16;14(45):50710-50717. doi: 10.1021/acsami.2c09729. Epub 2022 Nov 7.
All-solid-state Li metal batteries (ASSLBs) are currently regarded as one of the most promising next-generation energy storage technologies because of their great potential in realizing both high energy density and safety. However, the development of high performance ASSLBs is still restricted by the large interfacial resistance and Li dendrite propagation within solid electrolytes. Herein, a simple and efficient interfacial modification strategy is proposed to improve the interfacial contact between Li and LiLaZrTaO (LLZTO) by introducing a uniform and thin LiSe buffer layer. The LiSe buffer layer formed by an in situ conversion reaction can not only enhance the wettability of lithium metal toward LLZTO electrolyte but also facilitate uniform lithium plating/stripping. As a result, the interfacial resistance of Li/LLZTO decreased from 270.5 to 5.1 Ω cm, and the lithium symmetric cell can cycle stably for 350 h at a current density of 0.5 mA cm. Meanwhile, the Li|LLZTO-LiSe|LiNiCoMnO full cells exhibit a high initial capacity of 162.3 mAh g and good cycling stability with a capacity retention of 84.3% after 100 cycles at 0.2 C. These results prove the effectiveness of this modification method and provide new design strategies for the development of high performance ASSLBs.
全固态锂金属电池（ASSLBs）由于在实现高能量密度和安全性方面具有巨大潜力，目前被认为是最有前途的下一代储能技术之一。然而，高性能ASSLBs的发展仍然受到固体电解质内部大界面电阻和锂枝晶生长的限制。在此，提出了一种简单有效的界面修饰策略，通过引入均匀且薄的LiSe缓冲层来改善锂与LiLaZrTaO（LLZTO）之间的界面接触。通过原位转化反应形成的LiSe缓冲层不仅可以增强锂金属对LLZTO电解质的润湿性，还可以促进锂的均匀沉积/剥离。结果，Li/LLZTO的界面电阻从270.5降至5.1Ω·cm，锂对称电池在0.5 mA cm的电流密度下可以稳定循环350 h。同时，Li|LLZTO-LiSe|LiNiCoMnO全电池表现出162.3 mAh g的高初始容量和良好的循环稳定性，在0.2 C下100次循环后容量保持率为84.3%。这些结果证明了这种修饰方法的有效性，并为高性能ASSLBs的发展提供了新的设计策略。
