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 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.
