Interface Engineering of a Ceramic Electrolyte by Ta2O5 Nanofilms for Ultrastable Lithium Metal Batteries

• Published in: Advanced functional materials 2022-06, Vol.32 (24), p.n/a
• Main Authors: Guo, Sijie, Wu, Ting‐Ting, Sun, Yong‐Gang, Zhang, Si‐Dong, Li, Bing, Zhang, Hong‐Shen, Qi, Mu‐Yao, Liu, Xian‐Hu, Cao, An‐Min, Wan, Li‐Jun
• Format: Article
• Language: English
• Subjects: Anodes; Commercialization; coordination‐assisted deposition; Critical current density; Cycles; Electrode materials; Electrolytes; Energy storage; Interface stability; Interlayers; Lithium; Lithium batteries; lithium metal batteries; Materials science; Molten salt electrolytes; Solid electrolytes; solid‐state electrolytes; Storage batteries; surface modification; Ta 2O 5 nanofilm; Tantalum; Tantalum oxides
• ISSN: 1616-301X; 1616-3028
• DOI: 10.1002/adfm.202201498

Solid‐state batteries (SSBs) are promising for next‐generation energy storage with advantages in both energy density and safety, but are challenged by the poor solid‐to‐solid contact between solid‐state electrolytes (SSEs) and electrodes, particularly the lithium anode. Herein, a facile coordination‐assisted deposition process is employed to build artificial Ta2O5 nanofilms on SSEs, which is lithiophilic and has high stability against metallic lithium, thereby ensuring an intimate and stable interface between SSEs and lithium anode to sustain extended cycles. The feasibility is verified by using Li6.5La3Zr1.5Ta0.5O12 (LLZT), a garnet‐typed SSEs, as a model system. It is shown that a 12 nm Ta2O5 nanofilm is able to significantly decrease the interfacial resistance from 1258 to 9 Ω cm2 with a high critical current density reaching 2.0 mA cm−2 for the assembled symmetric cell, which shows an unprecedented capability to survive long‐term cycling over 5200 h. This control strategy is also able to enable the use of the commercialized cathode materials of LiFePO4 and LiNi0.83Co0.07Mn0.1O2 in SSBs with both high reversible capacity and cycling capability. The study opens up a research avenue for the delicately carved interlayers through a scalable and reliable manufacturing process which can accelerate the commercialization of SSEs. A coordination‐assisted deposition process is used to build an artificial Ta2O5 nanofilm onto garnet‐typed solid‐state electrolytes, which is highly efficient to address the interfacial challenge, and thereby ensures the significant decrease in interfacial resistance and extraordinary cycling capability of over 5200 h in Li metal batteries.