Multifunctional Glutathione Enables ISOS-Robust Inverted Perovskite Solar Cells via Dipole Engineering and Redox-Driven Self-Healing.

Abstract

Self-assembled monolayer (SAM)-based inverted perovskite solar cells (PSCs) suffer from a persistent efficiency-stability trade-off issue, which limits their commercialization. Herein, we propose a synergistic stabilizing strategy using reduced glutathione (GSH) as a multifunctional additive, integrating dipole modulation and redox-driven self-healing. GSH enables cross-scale regulation: inducing interfacial dipole via a concentration gradient, passivating bulk defects through Pb²⁺ coordination, optimizing crystallization kinetics, providing chemical protection against O₂•^- and moisture, and establishing a GSH/oxidized glutathione (GSSG)-Ni²⁺/Ni³⁺ redox cycle for self-healing at the NiO_x/SAM interface. Moreover, the interaction between GSSG and NiO_x opens an additional hole transport channel, effectively suppressing device performance degradation induced by ultraviolet (UV) irradiation and thermally-triggered cleavage of hydroxy groups in the SAM. Benefiting from the aforementioned advantages endowed by GSH, the small-area cell (4 mm²) achieved a high efficiency of 26.17%, while the 12.50 cm² minimodule reached 23.14%-among the highest values reported for modules with comparable active areas. Target devices also exhibit exceptional ISOS (International Summit on Organic Photovoltaic Stability) protocols stability: retaining 69.8% (ISOS-T-1, 200 h), 91.0% (ISOS-D-1, 1056 h), and 78.44% (ISOS-L-2, 336 h) of their initial efficiency. This work breaks the efficiency-stability trade-off and offers a "dynamic regulation-static protection" design principle for PSCs.