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

Coating Zr-based metallic glass, Zr53 Cu31 Ni11 Al5 (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.

2D PdTe2 Thin-Film-Coated Current Collectors for Long-Cycling Anode-Free Rechargeable Batteries.

The practical implementation of anode-free batteries is limited by factors such as lithium dendrite growth and low cycling Coulombic efficiency (CE). In this study, the improvement in the electrochemical performance of anode-free rechargeable lithium batteries bearing a Cu current collector (CC) coated with PdTe2 thin films is reported. The optimized thickness and sputtering heating conditions of the PdTe2 layer are 15 nm and 473.15 K, respectively. Upon deposition on a CC, PdTe2 works as a seed layer that considerably improves the CE in half-cells, owing to its unique 2D structure that reduces the nucleation overpotential. A further contribution to the high performance is brought about by a CuTe interphase between the coating layer and Cu CC formed during heating. Such an interphase contributes to the high CE by improving the uniformity of the current density distribution on the CC that suppresses lithium dendrite growth. A low nucleation overpotential and uniform current density distribution, in turn, result in a smooth morphology of the plated Li. The full cell obtained with the PdTe2-coated CC exhibits a capacity retention of 70.7% after the 100th cycle, with an average CE of 99.65% at a 0.2C rate─an outstanding result in view of the rapid development of lithium-ion batteries.