Organic-inorganic halide perovskites have significant potential for application in next-generation solar cells.However,their applications are limited by challenges associated with large-area processability and long-te...Organic-inorganic halide perovskites have significant potential for application in next-generation solar cells.However,their applications are limited by challenges associated with large-area processability and long-term stability owing to the presence of pinholes and defect sites.Here,we incorporated cesium formate in a perovskite active layer using a sequential perovskite fabrication process to eliminate the defect sites of perovskites and improve the film processability via roll-to-roll(R2R)processing.The addition of cesium formate salt to the PbI2 layer influences the perovskite crystal formation behavior as well as increases the perovskite crystallinity and decreases the defect density.Furthermore,cesium formate addition eliminated small PbI2 grains and smoothed the perovskite surface,resulting in a large crystal grain size.The formate ions interact with the PbI2 component and passivate halide vacancy defects,reducing nonradiative recombination and improving charge transfer.Additionally,the treated perovskite films were highly stable in air,exhibiting improved efficiency retention over time and achieving a power conversion efficiency(PCE)of>22%compared to the control.Furthermore,the additive-treated perovskite film was processed using the R2R method,achieving a high PCE of>14%with minimal hysteresis.展开更多
Organic-inorganic hybrid perovskite solar cells(PSCs)have emerged as a leading photovoltaic technology due to their exceptional power conversion efficiency(PCE)and low-cost fabrication process.However,the intrinsic th...Organic-inorganic hybrid perovskite solar cells(PSCs)have emerged as a leading photovoltaic technology due to their exceptional power conversion efficiency(PCE)and low-cost fabrication process.However,the intrinsic thermal instability of organic cations,such as methylammonium(MA^(+))and formamidinium(FA^(+)),necessitates their partial or complete substitution with inorganic cesium(Cs^(+))ions to enhance thermal robustness.While all-inorganic CsPbI_(3) exhibits superior thermal stability,its susceptibility to moisture and phase instability limits its practical applicability.Moreover,the toxicity of lead(Pb)has driven interest in tin(Sn)as a more sustainable alternative.In this study,we investigate the incorporation of pseudo-halide thiocyanate anions(SCN−)as a crystallization modulator for two-step spin-coating preparation of Cs_(0.1)FA_(0.9)Pb_(0.9)Sn_(0.1)I_(3) film,which promotes the formation of lead iodide coordination intermediates and lowering the energy barrier for perovskite crystal growth.By integrating Cs^(+)and Sn^(2+)into FAPbI_(3) perovskites with SCN−additives,the compositions,crystallinity,and grain interfaces of Cs_(0.1)FA_(0.9)Pb_(0.9)Sn_(0.1)I_(3) film are well tuned,yielding a PCE of 21.34%.The resulting PSCs demonstrated superior long-term stability and enhanced thermal resistance,highlighting the immense potential of SCN−mediated crystallization and tailored compositional engineering as effective strategies for the development of high-performance and thermally endurable PSCs.展开更多
Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious co...Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells(PSCs).In particular,the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films.Herein,we report the adoption of a pseudo-halide anion based ionic liquid additive,1-butyl-3-methylimidazolium thiocyanate(BMIMSCN)for growing ternary cation(CsFAMA,where FA=formamidinium and MA=methylammonium)perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening.Meanwhile,a novel halide-free passivator,benzylammonium formate(BAFa),was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination.As a result,the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime(from 79.41 to 201.01 ns),open-circuit voltage(from 1.13 to 1.19 V),photoelectric conversion efficiency(from 18.90%to 22.33%).Moreover,the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat.This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.展开更多
基金the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1C1C1012188),(No.2022M3J7A1066428)KK2352-20 funded by the Development of Platform Technology for Industrial Support based on Public-Infra.
文摘Organic-inorganic halide perovskites have significant potential for application in next-generation solar cells.However,their applications are limited by challenges associated with large-area processability and long-term stability owing to the presence of pinholes and defect sites.Here,we incorporated cesium formate in a perovskite active layer using a sequential perovskite fabrication process to eliminate the defect sites of perovskites and improve the film processability via roll-to-roll(R2R)processing.The addition of cesium formate salt to the PbI2 layer influences the perovskite crystal formation behavior as well as increases the perovskite crystallinity and decreases the defect density.Furthermore,cesium formate addition eliminated small PbI2 grains and smoothed the perovskite surface,resulting in a large crystal grain size.The formate ions interact with the PbI2 component and passivate halide vacancy defects,reducing nonradiative recombination and improving charge transfer.Additionally,the treated perovskite films were highly stable in air,exhibiting improved efficiency retention over time and achieving a power conversion efficiency(PCE)of>22%compared to the control.Furthermore,the additive-treated perovskite film was processed using the R2R method,achieving a high PCE of>14%with minimal hysteresis.
基金the financial support from the National Natural Science Foundation of China(Nos.22479074 and 22475096)the General Project of the Joint Fund of Equipment Pre-research and the Ministry of Education(No.8091B02052407)+7 种基金the Natural Science Foundation of Jiangsu Province(Nos.BK20240400 and BK20241236)the Science and Technology Major Project of Jiangsu Province(No.BG2024013)the Scientific and Technological Achievements Transformation Special Fund of Jiangsu Province(No.BA2023037)the Academic Degree and Postgraduate Education Reform Project of Jiangsu Province(No.JGKT24_C001)the Key Core Technology Open Competition Project of Suzhou City(No.SYG2024122)the open research fund of Suzhou Laboratory(No.SZLAB-1308-2024-TS005)the Gusu Leading Talent Program of Scientific and Technological Innovation and Entrepreneurship of Wujiang District in Suzhou City(No.ZXL2021273)the Chenzhou National Sustainable Development Agenda Innovation Demonstration Zone Provincial Special Project(No.2023sfq11).
文摘Organic-inorganic hybrid perovskite solar cells(PSCs)have emerged as a leading photovoltaic technology due to their exceptional power conversion efficiency(PCE)and low-cost fabrication process.However,the intrinsic thermal instability of organic cations,such as methylammonium(MA^(+))and formamidinium(FA^(+)),necessitates their partial or complete substitution with inorganic cesium(Cs^(+))ions to enhance thermal robustness.While all-inorganic CsPbI_(3) exhibits superior thermal stability,its susceptibility to moisture and phase instability limits its practical applicability.Moreover,the toxicity of lead(Pb)has driven interest in tin(Sn)as a more sustainable alternative.In this study,we investigate the incorporation of pseudo-halide thiocyanate anions(SCN−)as a crystallization modulator for two-step spin-coating preparation of Cs_(0.1)FA_(0.9)Pb_(0.9)Sn_(0.1)I_(3) film,which promotes the formation of lead iodide coordination intermediates and lowering the energy barrier for perovskite crystal growth.By integrating Cs^(+)and Sn^(2+)into FAPbI_(3) perovskites with SCN−additives,the compositions,crystallinity,and grain interfaces of Cs_(0.1)FA_(0.9)Pb_(0.9)Sn_(0.1)I_(3) film are well tuned,yielding a PCE of 21.34%.The resulting PSCs demonstrated superior long-term stability and enhanced thermal resistance,highlighting the immense potential of SCN−mediated crystallization and tailored compositional engineering as effective strategies for the development of high-performance and thermally endurable PSCs.
基金the National Key R&D Program of China(No.2017YFA0208200)the National Natural Science Foundation of China(Nos.22022505,21872069,and 22109069)+3 种基金the Fundamental Research Funds for the Central Universities of China(Nos.020514380266,020514380272,and 020514380274)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220008)the Nanjing International Collaboration Research Program(Nos.202201007 and 2022SX00000955)the Suzhou Gusu Leading Talent Program of Science and Technology Innovation and Entrepreneurship in Wujiang District(No.ZXL2021273).
文摘Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances,but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells(PSCs).In particular,the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films.Herein,we report the adoption of a pseudo-halide anion based ionic liquid additive,1-butyl-3-methylimidazolium thiocyanate(BMIMSCN)for growing ternary cation(CsFAMA,where FA=formamidinium and MA=methylammonium)perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening.Meanwhile,a novel halide-free passivator,benzylammonium formate(BAFa),was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination.As a result,the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime(from 79.41 to 201.01 ns),open-circuit voltage(from 1.13 to 1.19 V),photoelectric conversion efficiency(from 18.90%to 22.33%).Moreover,the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat.This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.
