A Self‐Reconfigured, Dual‐Layered Artificial Interphase Toward High‐Current‐Density Quasi‐Solid‐State Lithium Metal Batteries

• Published in: Advanced materials (Weinheim) Vol. 35; no. 24; pp. e2300350 - n/a
• Main Authors: Guo, Jun‐Chen, Tan, Shuang‐Jie, Zhang, Chao‐Hui, Wang, Wen‐Peng, Zhao, Yao, Wang, Fuyi, Zhang, Xu‐Sheng, Wen, Rui, Zhang, Ying, Fan, Min, Xin, Sen, Zhang, Juan, Guo, Yu‐Guo
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.06.2023
• Subjects: Anodes; artificial solid electrolyte interphase; Current density; Cycles; Electrolytic cells; lithiophilicity; Lithium; Lithium batteries; Lithium fluoride; lithium metal; Li‐ion transportation; Materials science; rechargeable batteries; Silver base alloys; Solid electrolytes; lithiophilicity; lithium metal; Li-ion transportation; rechargeable batteries; artificial solid electrolyte interphase
• ISSN: 0935-9648; 1521-4095; 1521-4095
• DOI: 10.1002/adma.202300350

The uncontrollable dendrite growth and unstable solid electrolyte interphase have long plagued the practical application of Li metal batteries. Herein, a dual‐layered artificial interphase LiF/LiBO–Ag is demonstrated that is simultaneously reconfigured via an electrochemical process to stabilize the lithium anode. This dual‐layered interphase consists of a heterogeneous LiF/LiBO glassy top layer with ultrafast Li‐ion conductivity and lithiophilic Li–Ag alloy bottom layer, which synergistically regulates the dendrite‐free Li deposition, even at high current densities. As a result, Li||Li symmetric cells with LiF/LiBO–Ag interphase achieve an ultralong lifespan (4500 h) at an ultrahigh current density and area capacity (20 mA cm−2, 20 mAh cm−2). LiF/LiBO–Ag@Li anodes are successfully applied in quasi‐solid‐state batteries, showing excellent cycling performances in symmetric cells (8 mA cm−2, 8 mAh cm−2, 5000 h) and full cells. Furthermore, a practical quasi‐solid‐state pouch cell coupling with a high‐nickel cathode exhibits stable cycling with a capacity retention of over 91% after 60 cycles at 0.5 C, which is comparable or even better than that in liquid‐state pouch cells. Additionally, a high‐energy‐density quasi‐solid‐state pouch cell (10.75 Ah, 448.7 Wh kg−1) is successfully accomplished. This well‐orchestrated interphase design provides new guidance in engineering highly stable interphase toward practical high‐energy‐density lithium metal batteries. A spontaneously reconfigured, dual‐layered artificial interphase of LiF/LiBO–Ag is proposed to stabilize Li anode at high current densities. The LiF/LiBO top layer guarantees fast Li‐ion transition, and the lithiophilic Li–Ag bottom layer enables uniform Li deposition. Benefiting from the well‐orchestrated interphase design, the quasi‐solid‐state lithium metal batteries demonstrate a high practical specific energy (448.7 Wh kg−1), superior high‐rate performances, and high safety.