Unlocking efficient photo-rechargeable Zn-Ion batteries via 1 T/2H MoS2 structural synergy and coupled intercalation/plating mechanism

In-situ 1 T/2H MoS 2 heterointerfaces synergistically combine 2H light-harvesting with 1 T conductivity for enhanced charge separation. • Optimized MoS 2 features expanded interlayer spacing and abundant active sites, accelerating Zn 2+ diffusion and redox kinetics. • The PRZIB delivers 340 mAh g −1 under illumination (vs. 237 mAh g −1 in dark) and achieves 1.2% photoconversion efficiency. • Photo-recharging couples Zn 2+ extraction with photoelectron-driven Zn deposition, while flexible devices demonstrate stable power output for LEDs. Photo-rechargeable Zn-ion batteries (PRZIBs) are constrained by photocathodes lacking efficient light harvesting, fast transport, and reversible Zn 2+ storage. Herein, we develop a temperature-controlled hydrothermal strategy to construct in-situ 1 T/2H MoS 2 photocathodes with tunable interlayer spacing and defect density. The optimized sample synthesized at 140 °C exhibits enlarged interlayer spacing, abundant active sites and an intimate 1 T/2H phase interface, which accelerate Zn 2+ diffusion and redox kinetics. Moreover, the semiconducting 2H domains absorb light while metallic 1 T domains extract photogenerated electrons, enabling synergistic charge separation. Consequently, the PRZIB achieves a photoconversion efficiency of 1.2% and a discharge capacity of 340 mAh g −1 under illumination, versus 237 mAh g −1 in the dark at 0.1 A g −1 . Mechanistically, quasi-in-situ XRD reveals that photo-recharging couples Zn 2+ extraction with photoelectron-driven Zn deposition, while discharge reverses via intercalation/stripping, as confirmed by reversible (002) reflections. Additionally, flexible devices demonstrate stable power output, driving a biomimetic bird and an LED. Overall, this work highlights heterophase junction engineering as a promising route for integrated photo-rechargeable systems.