While serious stability issues impede the commercialization of perovskite solar cells(PSCs),two-dime nsional(2D)perovskites based on fluorinated bulky cations have emerged as more intrinsically stable materials.Howeve...While serious stability issues impede the commercialization of perovskite solar cells(PSCs),two-dime nsional(2D)perovskites based on fluorinated bulky cations have emerged as more intrinsically stable materials.However,the influence of fluorination degree of the bulky aromatic cation on the per-formance of resulting PSCs has not been scrutinized.Here,2D perovskites(FxPEA)_(2)PbI_(4)(x=1,2,3,5)are grown in situ on the surface of the three-dime nsion al(3D)perovskite and dem on strate effective passivation of the surface defects of 3D perovskite.The power conversion efficiency(PCE)of the optimized devices were boosted from 20.75%for the control device to 21.09%,22.06%,22.74%and 21.86%for 2D/3D devices treated with 4-fluorophenethylamine iodide,3,5-difluorophenylethylamine iodide,2,4,5-trifluoroethylphenylethylamine iodide,and 1,2,3,4,5-pentafluorophenylethylamine iodide,respectively.We firstly reported two unexplored RP-type layered perovskites with F_(2)PEAI and F_(3)PEAI as bulky cations.The combined experimental and theoretical analysis revealed the reasons behind the various morphology,device performances,dynamic behavior,and humidity stability.The best performing F_(5)PEAI-treated device retaining 95.0%of its initial PCE under ambient atmosphere(with RH of 60%±5%)without encapsulation for 300 h storage.This work provides useful guidance for selecting fluorinated bulky cations with different molecular electronic properties,which will play an essential role in further improving the performance/stability of PSCs for the sake of further commercialization.展开更多
基金financial support from the National Natural Science Foundation of China (Grant No. 21975260)the financial support from the National Natural Science Foundation of China (Grant No. 22078241).
文摘While serious stability issues impede the commercialization of perovskite solar cells(PSCs),two-dime nsional(2D)perovskites based on fluorinated bulky cations have emerged as more intrinsically stable materials.However,the influence of fluorination degree of the bulky aromatic cation on the per-formance of resulting PSCs has not been scrutinized.Here,2D perovskites(FxPEA)_(2)PbI_(4)(x=1,2,3,5)are grown in situ on the surface of the three-dime nsion al(3D)perovskite and dem on strate effective passivation of the surface defects of 3D perovskite.The power conversion efficiency(PCE)of the optimized devices were boosted from 20.75%for the control device to 21.09%,22.06%,22.74%and 21.86%for 2D/3D devices treated with 4-fluorophenethylamine iodide,3,5-difluorophenylethylamine iodide,2,4,5-trifluoroethylphenylethylamine iodide,and 1,2,3,4,5-pentafluorophenylethylamine iodide,respectively.We firstly reported two unexplored RP-type layered perovskites with F_(2)PEAI and F_(3)PEAI as bulky cations.The combined experimental and theoretical analysis revealed the reasons behind the various morphology,device performances,dynamic behavior,and humidity stability.The best performing F_(5)PEAI-treated device retaining 95.0%of its initial PCE under ambient atmosphere(with RH of 60%±5%)without encapsulation for 300 h storage.This work provides useful guidance for selecting fluorinated bulky cations with different molecular electronic properties,which will play an essential role in further improving the performance/stability of PSCs for the sake of further commercialization.