Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surf...Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.展开更多
Poor wettability of poly(triarylamine)(PTAA)surfaces and insufficient control over residual PbI_(2) clusters remain critical bottlenecks limiting the performance of PTAA-based p-i-n perovskite solar cells(PSCs).Herein...Poor wettability of poly(triarylamine)(PTAA)surfaces and insufficient control over residual PbI_(2) clusters remain critical bottlenecks limiting the performance of PTAA-based p-i-n perovskite solar cells(PSCs).Herein,we introduce an effective interface engineering strategy through the incorporation of the ionic liquid 1-butyl-3-methylimidazolium acetate(BMIMAc).Owing to its strong affinity for the perovskite precursor solvent(N,N-dimethylformamide,DMF),BMIMAc significantly enhances PTAA wettability,promoting the formation of uniform and defect-passivated perovskite films.In addition,BMIMAc modulates the energy level alignment of PTAA,facilitating more efficient hole extraction and transport across the interface.More importantly,BMIMAc interacts with PbI_(2) to decelerate perovskite crystallization kinetics,enabling a more complete conversion of PbI_(2) into the perovskite phase.This synergistic regulation yields perovskite films with enlarged grain sizes,reduced trap densities,and suppressed nonradiative recombination losses.Benefiting from these advances,the optimized PTAA-based p-i-n PSCs achieve a record-high power conversion efficiency of 25.10%with significantly enhanced operational stability.展开更多
Nonionic poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA)-based inverted wide-bandgap perovskite solar cells(PSCs)are pivotal for advancing all-perovskite tandem architectures and indoor photovoltaics,yet their p...Nonionic poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA)-based inverted wide-bandgap perovskite solar cells(PSCs)are pivotal for advancing all-perovskite tandem architectures and indoor photovoltaics,yet their performance is fundamentally constrained by the hydrophobic nature of PTAA.Herein,we demonstrate a dual-interface molecular engineering strategy to synchronously modulate the perovskite-facing upper interface and substrate-contacting buried interface of PTAA using hydrophilic poly(methyl methacrylate)(PMMA)and poly(3-carboxypentyl thiophene)(P3 CT-N).The carbonyl(C=O)groups in PMMA and P3 CT-N synergistically enhance interfacial wettability,promoting the controlled crystallization of 1.78 eV widebandgap perovskites.Additionally,the carbonyl coordination effectively passivates undercoordinated Pb2+defects,improving charge transport dynamics.Meanwhile,vacuum-level shifting induced by the interface dipole of PMMA and P3 CT-N optimizes valence-band alignment,facilitating efficient hole extraction.As a result,the modified PTAA-based single-junction PSCs achieve a remarkable power conversion efficiency(PCE)of 19.38%under AM 1.5G illumination,significantly surpassing the17.06%of pristine PTAA devices.The sandwich polymer structure-based PTAA design further enhances indoor photovoltaic performance,yielding PCEs of 37.43% and 30.09% under 1000 lux and 200 lux LED illumination,respectively.Moreover,in allperovskite tandem configurations,the modified hole transport layer(HTL)enables a remarkable PCE of 26.87%under AM 1.5G illumination,outperforming control devices(25.38%).This strategy provides a robust pathway toward highly efficient and stable indoor and all-perovskite tandem photovoltaics based on wide-bandgap perovskite.展开更多
Polymer hole-transport layers(HTLs)are critical components of inverted perovskite solar cells(IPVSCs).Triphenylamine derivatives PTAA(poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine])and Poly-TPD(poly[N,N′-bis(4-butyl...Polymer hole-transport layers(HTLs)are critical components of inverted perovskite solar cells(IPVSCs).Triphenylamine derivatives PTAA(poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine])and Poly-TPD(poly[N,N′-bis(4-butylphenyl)-N,N′-bis(phenyl)benzidine])have been widely adopted as hole-transport materials due to their perovskite passivation effects and suitable energy levels.However,the passivation mechanism(i.e.,the functional group responsible for perovskite passivation)of triphenylamine derivative polymers remains unclear,hindering the development and application of this polymer type.Here,we develop a novel Poly-TPD derivative,S-Poly-TPD,by replacing the n-butyl functional group of Poly-TPD with an isobutyl group to explore the influence of alkyl groups on HTL performance and top-deposited perovskite properties.Compared with Poly-TPD,the increased CH_(3)-terminal unit density and the decreased spatial distance between the-CH-CH_(3) and-CH_(2)-CH_(3) units and the benzene ring in S-Poly-TPD not only enhanced the hole-transport ability but also improved the perovskite passivation effect,revealing for the first time the role of the alkyl groups in perovskite passivation.As a result,the S-Poly-TPD-based IPVSCs demonstrated high power-conversion efficiencies of 15.1% and 21.3% in wide-bandgap[MAPbI_(2)Br(SCN)0.12]and normal-bandgap[(FAPbI_(3))0.92(MAPbBr_(3))0.08]devices,respectively.展开更多
基金supported by the Research Projects of the Department of Education of Guangdong Province 2024ZDZX3079The financial support from the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011677)+4 种基金the Scientific and Technical Innovation Council of Shenzhen(20220812165832002)the Research Projects of Department of Education of Guangdong Province-2023GCZX015the Innovation Team Project of Guangdong(2022KCXTD055)the China Postdoctoral Science Foundation(Certificate Number:2024M763441)is gratefully acknowledgedsupported by the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20250031 and Research Projects of the Department of Education of Guangdong Province 2023GCZX015。
文摘Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.
基金funded by Nazarbayev University under Collaborative Research Program(Grant No.211123CRP1613,A.N.)Faculty Development Competitive Research Grants Program for 2024-2026(Grant No.201223FD8801,A.N.)+5 种基金This work is supported by Scientific Research Startup Fund for Spray-on Perovskite Photovoltaics R&D Center(No.602331011PQ)Research Projects of Department of Education of Guangdong Province 2024ZDZX3079The financial support from Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011677)the Scientific and Technical Innovation Council of Shenzhen(20220812165832002)Research Projects of Department of Education of Guangdong Province-2023GCZX015the Innovation Team Project of Guangdong(2022KCXTD055)is gratefully acknowledged.Q.L.and F.W.contributed equally to this work.
文摘Poor wettability of poly(triarylamine)(PTAA)surfaces and insufficient control over residual PbI_(2) clusters remain critical bottlenecks limiting the performance of PTAA-based p-i-n perovskite solar cells(PSCs).Herein,we introduce an effective interface engineering strategy through the incorporation of the ionic liquid 1-butyl-3-methylimidazolium acetate(BMIMAc).Owing to its strong affinity for the perovskite precursor solvent(N,N-dimethylformamide,DMF),BMIMAc significantly enhances PTAA wettability,promoting the formation of uniform and defect-passivated perovskite films.In addition,BMIMAc modulates the energy level alignment of PTAA,facilitating more efficient hole extraction and transport across the interface.More importantly,BMIMAc interacts with PbI_(2) to decelerate perovskite crystallization kinetics,enabling a more complete conversion of PbI_(2) into the perovskite phase.This synergistic regulation yields perovskite films with enlarged grain sizes,reduced trap densities,and suppressed nonradiative recombination losses.Benefiting from these advances,the optimized PTAA-based p-i-n PSCs achieve a record-high power conversion efficiency of 25.10%with significantly enhanced operational stability.
基金supported by the National Natural Science Foundation of China(62205142,22425903,U24A20568,61705102,62288102,222409091,22409090)the National Key R&D Program of China(2023YFB4204500,2020YFA07099003)the Jiangsu Provincial Department of Science and Technology(BE2022023,BK20220010,BZ2023060,BK20241875)。
文摘Nonionic poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA)-based inverted wide-bandgap perovskite solar cells(PSCs)are pivotal for advancing all-perovskite tandem architectures and indoor photovoltaics,yet their performance is fundamentally constrained by the hydrophobic nature of PTAA.Herein,we demonstrate a dual-interface molecular engineering strategy to synchronously modulate the perovskite-facing upper interface and substrate-contacting buried interface of PTAA using hydrophilic poly(methyl methacrylate)(PMMA)and poly(3-carboxypentyl thiophene)(P3 CT-N).The carbonyl(C=O)groups in PMMA and P3 CT-N synergistically enhance interfacial wettability,promoting the controlled crystallization of 1.78 eV widebandgap perovskites.Additionally,the carbonyl coordination effectively passivates undercoordinated Pb2+defects,improving charge transport dynamics.Meanwhile,vacuum-level shifting induced by the interface dipole of PMMA and P3 CT-N optimizes valence-band alignment,facilitating efficient hole extraction.As a result,the modified PTAA-based single-junction PSCs achieve a remarkable power conversion efficiency(PCE)of 19.38%under AM 1.5G illumination,significantly surpassing the17.06%of pristine PTAA devices.The sandwich polymer structure-based PTAA design further enhances indoor photovoltaic performance,yielding PCEs of 37.43% and 30.09% under 1000 lux and 200 lux LED illumination,respectively.Moreover,in allperovskite tandem configurations,the modified hole transport layer(HTL)enables a remarkable PCE of 26.87%under AM 1.5G illumination,outperforming control devices(25.38%).This strategy provides a robust pathway toward highly efficient and stable indoor and all-perovskite tandem photovoltaics based on wide-bandgap perovskite.
基金The work was financially supported by the Guangdong Major Project of Basic and Applied Basic Research(No.2019B030302007)the Ministry of Science and Technology(Nos.2017YFA0206600,2019YFA 0705900)+3 种基金the Natural Science Foundation of China(Nos.51973063,91733302 and 51803060)the Science and Technology Program of Guangdong Province,China(No.2018A030313045)the Science and Technology Program of Guangzhou,China(No.201904010147).Yue‐Min Xie acknowledged the funding by State Key Lab of Luminescent Materials and Devices,South China Uni-versity of Technology,the Fellowship of China Post-doctoral Science Foundation(No.2020M682703)the National Natural Science Foundation of China(No.52003090).
文摘Polymer hole-transport layers(HTLs)are critical components of inverted perovskite solar cells(IPVSCs).Triphenylamine derivatives PTAA(poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine])and Poly-TPD(poly[N,N′-bis(4-butylphenyl)-N,N′-bis(phenyl)benzidine])have been widely adopted as hole-transport materials due to their perovskite passivation effects and suitable energy levels.However,the passivation mechanism(i.e.,the functional group responsible for perovskite passivation)of triphenylamine derivative polymers remains unclear,hindering the development and application of this polymer type.Here,we develop a novel Poly-TPD derivative,S-Poly-TPD,by replacing the n-butyl functional group of Poly-TPD with an isobutyl group to explore the influence of alkyl groups on HTL performance and top-deposited perovskite properties.Compared with Poly-TPD,the increased CH_(3)-terminal unit density and the decreased spatial distance between the-CH-CH_(3) and-CH_(2)-CH_(3) units and the benzene ring in S-Poly-TPD not only enhanced the hole-transport ability but also improved the perovskite passivation effect,revealing for the first time the role of the alkyl groups in perovskite passivation.As a result,the S-Poly-TPD-based IPVSCs demonstrated high power-conversion efficiencies of 15.1% and 21.3% in wide-bandgap[MAPbI_(2)Br(SCN)0.12]and normal-bandgap[(FAPbI_(3))0.92(MAPbBr_(3))0.08]devices,respectively.
