Forming Robust and Highly Li‐Ion Conductive Interfaces in High‐Performance Lithium Metal Batteries Using Chloroethylene Carbonate Additive

Abstract

Developing high‐rate Li metal batteries (LMBs) is challenging because of dendrite growth and irreversible parasitic reactions of the Li metal. Herein, a robust and highly ion‐conductive solid electrolyte interphase (SEI) layer is designed on a Li metal anode and a Ni‐rich layered cathode by incorporating chloroethylene carbonate (ClEC) as an additive in fluoroethylene carbonate‐based electrolytes. ClEC induces the formation of LiCl, which facilitates Li‐ion diffusion in the robust LiF‐rich SEI layer, thereby improving the cycle stability of the Li metal anode and suppressing microcracking of the Ni‐rich layered cathode, especially during charging and discharging at high current densities. By using the newly developed combination of electrolyte solution, an LMB featuring the Li[Ni0.78Co0.1Mn0.12]O2 cathode (2.3 mAh cm−2, 0.1 C) affords a superior capacity retention of 80.2% over 400 cycles at high charge and discharge current densities of 2.0 C (3.6 mA cm−2) and 5.0 C (9.0 mA cm−2). This study provides insights into the use of ClEC as an electrolyte additive and highlights the importance of constructing robust and highly ion‐conductive interfaces on both Li metal anodes and Ni‐rich cathodes for high‐performance LMBs.

A Review of Macrocycles Applied in Electrochemical Energy Storge and Conversion

“…Rechargeable batteries and supercapacitors play major roles in energy storage and conversion devices [ 3 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 ]; the working mechanism of these devices is illustrated in Figure 1 . Moreover, tremendous efforts have been devoted to advancing these high-performance energy storage and conversion devices, aiming for enhanced capacity, power density, and cycle life [ 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 , 23 ]. For instance, the utilization of lithium-ion batteries (LIBs) in our daily lives has significantly increased since the 1990s, with a notable achievement of achieving a high energy density of approximately 250 Wh kg −1 with an extended cycling life more than 1000 cycles [ 24 , 25 , 26 , 27 ].…”