All-Solid-State Thin-Film Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice. However, the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into all-solid-state thin-film batteries, leading to inexperience in fabricating all-solid-state thin-film Li-S batteries (TFLSBs). Herein, for the first time, TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S (VGs-Li2S) composite thin-film cathode, lithium-phosphorous-oxynitride (LiPON) thin-film solid electrolyte, and Li metal anode. Fundamentally eliminating Li-polysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an "unlimited Li" reservoir, which exhibits excellent long-term cycling stability with a capacity retention of 81% for 3,000 cycles, and an exceptional high temperature tolerance up to 60 °C. More impressively, VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%. Collectively, this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.

Vertical Graphene Film Enables High-Performance Quasi-Solid-State Planar Zinc-Ion Microbatteries.

With the advantages of low cost, high safety, and environmental friendliness, quasi-solid-state zinc-ion microbatteries (ZIMBs) have received widespread attention in the field of flexible wearable devices and on-chip integratable energy storage. However, hysteresis Zn-ion transport kinetics and inhomogeneous growth of the zinc anode result in the poor capacity reversibility and cycling stability. Herein, a quasi-solid-state planar zinc-ion cell was developed by employing a vertical graphene (VG) film as an effective conductive modification layer for both the cathode and anode. The VG distinctly induces uniform Zn deposition/stripping, accelerates the charge transport, and enhances the adhesion between the active materials and current collectors. As a result, planar Zn@VG//MnO2@VG exhibits a high areal capacity of 159 µAh cm-2, a remarkably high areal energy/power density of 201.5 µWh cm-2/67.16 µW cm-2, and a high capacity retention of 95.6% at a bending angle of 180°. The proposed facile strategy for electrode modification provides a new insight into the design of high-performance flexible and planar ZIMBs.