Defects-Triggered In Situ Reconstruction in Metal-Halide Perovskites for Photo-Rechargeable Lithium-Ion Batteries

Abstract

Photo-rechargeable batteries (PRBs), which refer to the integrated energy conversion-storage units, are receiving intense interest as they are able to solve the drawbacks in the traditional off-grid supply system (e.g., intermittency of solar energy, ohmic losses by wire-connection, and voltage mismatch). Bifunctional photoelectrodes, which are active materials with both photovoltaic and energy-storage capabilities, are the key matrices in PRBs. Herein, a bifunctional photoelectrode with heterojunctions based on lead-free metal-halide perovskites (MHPs) is formed via a spontaneous two-step reconstruction triggered by octahedral defects and arrangement. Due to the partial dissolution of octahedra (e.g., [SnI₆]²⁻ or [Bi₂I₉]³⁻) in N-methyl-2-pyrrolidone solution during fabrication of electrodes, the Cu current collector is reactivated with the Cu⁺/Cu²⁺ leaching, thereby enabling the in situ formation of CuO (CuI)/MHPs heterojunctions, which significantly enhances the conductivity of the photoelectrodes and effectively improves the stability. The reconstructed electrodes deliver remarkable specific capacity in both photo-assisted (684.6 mAh g⁻¹ at 0.6 A g⁻¹) and photo-charge (0.316 mAh cm⁻² at 2 mA cm⁻²) conditions, as well as the integrated micro-PRLIBs show all-day applications in wearable electronics. This work provides a generalizable framework for constructing efficient photo-rechargeable systems with high integration for wearable and portable devices, such as smart textiles and biosensors.

Keywords

B-site defects / metal-halide perovskites / octahedral arrangement / photo-rechargeable batteries / reconstruction

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