Exploiting Zirconium‐Based Metallic Glass Thin Films for Anode‐Free Lithium‐Ion Batteries and Lithium Metal Batteries With Ultra‐Long Cycling Life

Abstract

AbstractCoating Zr‐based metallic glass, Zr53Cu31Ni11Al5 (Zr‐MG), on a Cu current collector (CC) and Li metal anode (LMA) significantly improves the cycle performance of both types of Li‐ion batteries, namely, anode‐free Li‐ion batteries (AFLBs) and Li metal batteries (LMB). The inherent isotropy and homogeneity of the Zr‐MG significantly improve the surface uniformity of the CC and LMA. A 12 nm‐thick Zr‐MG thin film coating on the CC reduces the overpotential in the AFLB, leading to a more uniform Li plating morphology. The Li film covers almost the entire surface of the Zr‐CC, whereas it only covers ≈75% of the bare CC during charging. An LFP||Zr‐CC full‐cell exhibits a capacity retention of 63.6% after the 100th cycle, with an average CE of 99.55% at a 0.2 C rate. In the case of the LMB, a 12 nm‐thick Zr‐MG thin film‐coated LMA (Zr‐LMA) exhibits a stable capacity of up to 1500 cycles. An LFP||Zr‐LMA full‐cell exhibits capacity retention and CE after 1500 cycles of 66.6% and 99.97%, respectively, at a 1 C rate. Zirconium‐MG thin films with atomic‐level uniformity, outstanding corrosion resistance, lithiophilic characteristics, and high diffusivity result in superior AFLB and LMB performances.