Breaking the Efficiency-Stability-Sustainability Trilemma in all-perovskite Tandem Solar Modules via Oxidative...

Narrow-bandgap (NBG) tin-lead (Sn-Pb) perovskites are vital for all-perovskite tandem solar modules (TSMs), yet their commercialization remains limited by challenges in balancing efficiency, stability, and sustainability. Here, we presented an oxidation-triggered blockchain molecular (BCM) interface engineering strategy, which modified the poly (3,4-ethylenedioxythiophene):poly (styrene sulfonate) (PEDOT:PSS) surface and constructed a dynamic functional layer at the buried PEDOT:PSS/Sn-Pb perovskite interface through synergistic effects of biocompatible rutin molecules and their oxidation derivatives. This approach enabled full-cycle optimization from film formation to operational longevity via sequential regulation of crystallization and carrier dynamics, along with persistent defect passivation through synergistic coordination and hydrogen bonding. Resulting NBG devices achieved champion efficiencies of 23.50% (0.045 cm²) and 17.10% (10.4 cm²), respectively. The all-perovskite TSMs (10.4 cm²) attained a 23.00% aperture efficiency (an active-area efficiency of 24.30%) and retained ∼90% efficiency after 640 h of continuous illumination (extrapolated T_PCE80 lifetime of 3900 h) and after 15 cycles of day-night fatigue tests. Additionally, BCM's dual protection effects (physical barrier and chemical chelation) reduced lead leakage of severely damaged TSMs by 90% under simulated heavy rainfall, demonstrating strong environmental resilience. This work offers a scalable molecular strategy for advancing perovskite photovoltaics from lab-scale innovation to industrial viability.