The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement rema...The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.展开更多
The replacement of small cations with bulkier organic cations containing long alkyl chains or benzene rings to form a thin two-dimensional(2D)perovskite passivation layer on three-dimensional(3D)perovskite(2D/3D)has b...The replacement of small cations with bulkier organic cations containing long alkyl chains or benzene rings to form a thin two-dimensional(2D)perovskite passivation layer on three-dimensional(3D)perovskite(2D/3D)has become a promising strategy for improving both the efficiency and stability of perovskite solar cells(PSCs).The 2 D layer defines the interfacial chemistry and physics at the 2D/3D bilayer and endows the 2D/3D structure with better chemical and thermal stability.Herein,2D/3D(CF_(3)-PEA)_(2) FA_(0.85)MA_(0.15)Pb_(2)I_(7)/FA_(0.85)MA_(0.15)PbI_(3) planar heterojunction perovskite was produced using a facile interfacial ion exchange process.The 2 D(CF_(3)-PEA)_(2) FA_(0.85)MA_(0.15)Pb_(2)I_(7) capping layer can not only passivate the FA_(0.85)MA_(0.15)PbI_(3) film but also act as super-hydrophobic layer to inhibit water diffusion and significantly enhance the stability.The 2D capping layer can also establish a unique graded band structure at the perovskite/Spiro-OMeTAD interface and lead to p-type doping for Spiro-OMeTAD layer which is beneficial for efficient charge transport.Optimized PSCs based on this 2D/3D heterojunction yield a champion power conversion efficiency(PCE)of 23.1%and improved stability.The device maintains 84%output for 2400 h aging under ambient environmental conditions without encapsulation,and maintains 81%for 200 h under illumination with encapsulation.This work will inspire the design of more fluorinated 2D perovskite interfaces for advanced photovoltaics and beyond.展开更多
基金support from the National Natural Science Foundation of China(62074095)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities(GK202002001)the 111 Project(Grant No.B21005)the DNL Cooperation Fund CAS(DNL180311)the support of H2 cluster in Xi’an Jiaotong University.
文摘The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.
基金support from the National Natural Science Foundation of China(62074095)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities(GK202002001)the 111 Project B(14041)the DNL Cooperation Fund CAS(DNL180311)support of the H2 cluster in Xi’an Jiaotong University。
文摘The replacement of small cations with bulkier organic cations containing long alkyl chains or benzene rings to form a thin two-dimensional(2D)perovskite passivation layer on three-dimensional(3D)perovskite(2D/3D)has become a promising strategy for improving both the efficiency and stability of perovskite solar cells(PSCs).The 2 D layer defines the interfacial chemistry and physics at the 2D/3D bilayer and endows the 2D/3D structure with better chemical and thermal stability.Herein,2D/3D(CF_(3)-PEA)_(2) FA_(0.85)MA_(0.15)Pb_(2)I_(7)/FA_(0.85)MA_(0.15)PbI_(3) planar heterojunction perovskite was produced using a facile interfacial ion exchange process.The 2 D(CF_(3)-PEA)_(2) FA_(0.85)MA_(0.15)Pb_(2)I_(7) capping layer can not only passivate the FA_(0.85)MA_(0.15)PbI_(3) film but also act as super-hydrophobic layer to inhibit water diffusion and significantly enhance the stability.The 2D capping layer can also establish a unique graded band structure at the perovskite/Spiro-OMeTAD interface and lead to p-type doping for Spiro-OMeTAD layer which is beneficial for efficient charge transport.Optimized PSCs based on this 2D/3D heterojunction yield a champion power conversion efficiency(PCE)of 23.1%and improved stability.The device maintains 84%output for 2400 h aging under ambient environmental conditions without encapsulation,and maintains 81%for 200 h under illumination with encapsulation.This work will inspire the design of more fluorinated 2D perovskite interfaces for advanced photovoltaics and beyond.