• A natural and regenerable redox shuttle using glutathione (GSH) effectively eliminates harmful Sn4+ and Sn0/Pb0 impurities in Pb-Sn perovskite solar cells.
• GSH incorporation regulates perovskite crystallization, leading to high-quality charge separation junctions and improved device performance.
• GSH-modified Pb-Sn solar cells achieve a champion PCE of 23.71%, and all-perovskite tandem cells reach 28.49% with 90% retention after 560 hours.
• This nature-inspired redox shuttling strategy provides a new pathway for developing efficient and stable all-perovskite tandem solar cells.
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