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Breaking the Efficiency‐Stability‐Sustainability Trilemma in all‐perovskite Tandem Solar Modules via Oxidative Blockchain Molecular Engineering

Guo YangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaJinglin SunSchool of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 P. R. ChinaXueqing ChangInstitute of Innovation Materials and Energy School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 P. R. ChinaChao YuSchool of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 P. R. ChinaGengling LiuCollege of Chemistry and Materials Science Gannan Normal University Ganzhou 341000 P. R. ChinaYuxuan FangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaHuanyu ChenKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaYuhua HuangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaHong LiuKey Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of New Energy and Electrical Engineering Hubei University Wuhan 430062 P. R. ChinaJun FangDepartment of Mechanical and Energy Engineering SUSTech Energy Institute for Carbon Neutrality Southern University of Science and Technology Shenzhen 518055 P. R. ChinaLixiang WangState Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310027 P. R. ChinaYing TanKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaWenhuai FengKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaMeifang YangInstitute of Innovation Materials and Energy School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 P. R. ChinaYongbin FengKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaJun‐Xing ZhongSchool of Chemistry and Materials Science Guangdong University of Education Guangzhou 510303 P. R. ChinaD. D. GulamovaUzbekistan Academy of Sciences Institute of Materials Science Chingiz Aytmatov str.2B Tashkent 100084 UzbekistanYanjun FangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaCongcong WuKey Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer Materials School of New Energy and Electrical Engineering Hubei University Wuhan 430062 P. R. ChinaLongbin QiuDepartment of Mechanical and Energy Engineering SUSTech Energy Institute for Carbon Neutrality Southern University of Science and Technology Shenzhen 518055 P. R. ChinaXudong WangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. ChinaZhibin YangSchool of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 P. R. ChinaWu‐Qiang WuKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFM School of Chemistry IGCME Sun Yat‐Sen University Guangzhou 510275 P. R. China
Advanced Materialsjournal2025en
ABI

Abstract

Abstract 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 cm 2 ) and 17.10% (10.4 cm 2 ), respectively. The all‐perovskite TSMs (10.4 cm 2 ) 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.

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