Yao‐Xian WangShih‐Kuan HongHsiao‐Ping HsuCHUNG-WEN LAN2024-07-092024-07-092024-06https://www.scopus.com/record/display.uri?eid=2-s2.0-85194552977&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/719678Anode-free lithium metal batteries have attracted much attention due to their high energy density and lack of excess Li. In this work, Li film is deposited on large-area copper foil (64 cm2) with good uniformity by a self-designed electroplating device that quickly assembles and can be operated outside the glove box. By adding the high concentration of LiNO3 into the lithium bis(trifluoromethylsulfonyl)azanide (LiTFSI)-based electrolyte, the high Li+ conductive solid electrolyte interface (SEI) layer regulated the Li+ flux, forming the columnar structure at a high current density of 40 mA cm−2, and compact morphology at 60 mA cm−2. Even at 100 mA cm−2, Li film on copper foil (Li@Cu) maintains its macroscopic uniformity. Furthermore, electrolytes, additives, and temperature are further optimized. The symmetric Li@Cu || Li cell cycle life can extend to 80 cycles. This work provides essential information for future manufacturing processes and scale-up.falsecolumnar Li Structurehigh current densityhigh Li+ conductive SEI layerlithiumthin filmsjournal article10.1002/admt.2024001162-s2.0-85194552977