Buried-Interface Iodine Redox Regulation for Durable All-Perovskite Tandem Photovoltaics

Tin-lead (Sn-Pb) mixed perovskites have propelled all-perovskite tandem solar cells (APTSCs) beyond 30% efficiency, yet buried-interface instability impedes commercialization. The ubiquitous PEDOT:PSS layer readily facilitates the oxidation of I^-, and the subsequent diffusion of corrosive I₂ severely compromises device performance-a fundamental chemical degradation pathway that leaves unresolved. Here, we introduce 6-amino-2-thiouracil (ATU) as a multifunctional additive that chemically targets this degradation pathway. Embedded within the PEDOT:PSS layer, the interaction between ATU and PSS contributes to alleviating the oxidation of I^- while its C═S moiety actively reduces corrosive I₂ back to I^-, establishing a dynamic iodine-recycling mechanism that addresses the root chemical cause of instability. Concurrent defect passivation and crystallization modulation further enhance film quality. Benefiting from these synergistic effects, the optimized APTSCs achieve a champion efficiency of 29.29% (certified 28.79%) and exhibit significantly improved stability, maintaining over 85% of their initial efficiency after 500 h of maximum power point tracking. By targeting buried-interface corrosive I₂, this work provides a rational framework beyond conventional passivation for durable perovskite photovoltaics.