FAPbI3 has been extensively employed in high-performance perovskite solar cells(PSCs)owing to its optimal bandgap and outstanding optoelectronic properties.Nevertheless,it readily undergoes the formation of a photo-in...FAPbI3 has been extensively employed in high-performance perovskite solar cells(PSCs)owing to its optimal bandgap and outstanding optoelectronic properties.Nevertheless,it readily undergoes the formation of a photo-inactiveδ-phase during crystallization,and achieving high-qualityα-phase films becomes even more challenging in antisolvent-free fabrication processes.This study introduces a crystallization control strategy based on 2-dimethylaminopyridine(2-DMAP)ligand engineering to establish a“fast nucleation-slow growth”dual-time-domain crystallization mechanism.2-DMAP facilitates the formation of a functional intermediate phase(2-DMAP·PbI_(2)·DMSO)that enables a direct transformation to theα-FAPbI3 phase and effectively suppresses theδ-phase pathway.Theoretical calculations and systematic experimental characterizations demonstrate that 2-DMAP exhibits stronger binding affinity and a greater charge polarization effect than dimethylsulfoxide(DMSO).This promotes the formation of high-density nuclei during spin coating and delays excessive grain growth during annealing,leading to perovskite films with improved crystallinity,fewer defects,and longer carrier lifetimes.As a result,an antisolvent-free PSC device was successfully fabricated,achieving a power conversion efficiency(PCE)of 25.10%,one of the highest reported for antisolvent-free spin-coating systems.Under ISOS-L-1 standard conditions,the device retained 84.78%of its initial efficiency after 1500 h of continuous illumination,demonstrating excellent operational stability.Moreover,it exhibited remarkable long-term stability under harsh humid and thermal conditions.This work offers a valuable strategy for the large-scale fabrication of high-performance and antisolvent-free PSCs.展开更多
基金supported by the National Natural Science Foundation of China (62374104, 62374103)the Taishan Scholar Foundation of Shandong Province (tsqn2023120051105)+1 种基金the Natural Science Foundation of Shandong Province (ZR2023QE321)the Shandong University-Muerhls Joint Laboratory
文摘FAPbI3 has been extensively employed in high-performance perovskite solar cells(PSCs)owing to its optimal bandgap and outstanding optoelectronic properties.Nevertheless,it readily undergoes the formation of a photo-inactiveδ-phase during crystallization,and achieving high-qualityα-phase films becomes even more challenging in antisolvent-free fabrication processes.This study introduces a crystallization control strategy based on 2-dimethylaminopyridine(2-DMAP)ligand engineering to establish a“fast nucleation-slow growth”dual-time-domain crystallization mechanism.2-DMAP facilitates the formation of a functional intermediate phase(2-DMAP·PbI_(2)·DMSO)that enables a direct transformation to theα-FAPbI3 phase and effectively suppresses theδ-phase pathway.Theoretical calculations and systematic experimental characterizations demonstrate that 2-DMAP exhibits stronger binding affinity and a greater charge polarization effect than dimethylsulfoxide(DMSO).This promotes the formation of high-density nuclei during spin coating and delays excessive grain growth during annealing,leading to perovskite films with improved crystallinity,fewer defects,and longer carrier lifetimes.As a result,an antisolvent-free PSC device was successfully fabricated,achieving a power conversion efficiency(PCE)of 25.10%,one of the highest reported for antisolvent-free spin-coating systems.Under ISOS-L-1 standard conditions,the device retained 84.78%of its initial efficiency after 1500 h of continuous illumination,demonstrating excellent operational stability.Moreover,it exhibited remarkable long-term stability under harsh humid and thermal conditions.This work offers a valuable strategy for the large-scale fabrication of high-performance and antisolvent-free PSCs.
