The inevitable ion migration that occurs within ionic polycrystalline perovskite film results in inferior longterm stability of perovskite solar cells(PVSCs)that cannot meet the commercial requirements.Here,a novel po...The inevitable ion migration that occurs within ionic polycrystalline perovskite film results in inferior longterm stability of perovskite solar cells(PVSCs)that cannot meet the commercial requirements.Here,a novel poly(ionic liquid)named poly-1-vinyl-3-propyltrimethoxysilane imidazolium chloride(PImIL-SiO)is first introduced into perovskite to strengthen grain boundaries(GBs)and construct dual-functional barriers against internal ion migration and external moisture erosion for fabricating highly efficient and stable PVSCs.PImIL-SiO-containing imidazoliumcations and pendant siloxane groups contribute to passivation of bulk defects and anchoring of GBs,which effectively hinders ion migration channels,thus reducing perovskite film phase separation and device hysteresis.Furthermore,the intrinsically hydrophobic PImIL-SiO automatically forms a secondary protective barrier to endow the perovskite film with ultrahigh moisture corrosion resistance through the hydrolyzation reaction of siloxane with the permeated moisture.Consequently,the PImIL-SiO-modified PVSCs achieve a champion power conversion efficiency(PCE)of 22.46%,accompaniedby excellent thermal andhumidity stabilities where the non-encapsulated devices retain 87%of the initial PCE after aging at 85℃for 250 h and>85%of the initial PCE over 1100 h in air with a relative humidity of 50–70%.展开更多
The novel triplet–triplet annihilation(TTA)upconversion(UC)field of rubrene(Rub)and dibenzotetraphenylperiflanthene(DBP)sensitized by bulk metal halide perovskite,integrated with copper-2,3,9,10,16,17,23,24-octafluor...The novel triplet–triplet annihilation(TTA)upconversion(UC)field of rubrene(Rub)and dibenzotetraphenylperiflanthene(DBP)sensitized by bulk metal halide perovskite,integrated with copper-2,3,9,10,16,17,23,24-octafluorophthalocyanine(F_(8)CuPc)as cosensitizer,have been investigated in perovskite solar cells(PVSCs)to minimize sub-bandgap photon transmission loss.The firm hydrogen bonding interaction(F…H–N between F_(8)CuPc and MA+),cation-πinteraction(MA+with Rub),and the hydrophobic characteristic of additives enable F_(8)CuPc:Rub:DBP dually-sensitized p-i-n PVSCs based on MAPbI_(3)and Cs_(0.05)(FA_(0.83)MA_(0.17))_(0.95)Pb(Br_(0.17)I_(0.83))_(3)absorbers to attain champion efficiencies of 20.83%and 21.51%,respectively.Furthermore,due to the excellent photochemical and thermal stability of F_(8)CuPc,the corresponding PVSCs can maintain nearly 80%of the original efficiencies exposed to air with 50∼70%relative humidity over 1100 h and N_(2)at 85℃for 300 h.展开更多
SrTiO_(3)-based oxides have been investigated as a promising n-type thermoelectric material at high temperatures;however,the relatively high thermal conductivity results in inferior thermoelectric performance.The latt...SrTiO_(3)-based oxides have been investigated as a promising n-type thermoelectric material at high temperatures;however,the relatively high thermal conductivity results in inferior thermoelectric performance.The lattice thermal conductivity can be significantly reduced by high-entropy engineering via severe lattice distortion.However,high configuration entropy also causes the deterioration of carrier mobility and restrains electron transport resulting in low electrical conductivity.In this work,the low lattice thermal conductivity of 1.7 W/(m·K)at 1073 K and significantly improved electrical conductivity of 112 S/cm from 60 S/cm can be achieved in n-type(Sr_(0.25)Ca_(0.25)Ba_(0.25)La_(0.25))TiO_(3)/Pb@Bi composites ceramics with core-shell grains of all-scale hierarchical microstructure.The effects of the complex microstructure of core-shell grains as well as the precipitated Pb@Bi particles on electrons and phonons transport properties were systematically explored.ZTmax of 0.18 was obtained for the SPS-1200,which was 1.5 times that of pure high-entropy(Ca_(0.2)Sr_(0.2)Ba_(0.2)La_(0.2)Pb_(0.2))TiO_(3)samples prepared by a solid-state method.This improvement in thermoelectric performance contributes to the addition of Bi_(2)O_(3)into the high-entropy(Sr_(0.2)Ca_(0.2)Ba_(0.2)Pb_(0.2)La_(0.2))TiO_(3)matrix resulting in multiphase core-shell grain structure combined with well-dispersed nano-sized metal Pb@Bi precipitates in the matrix.This feasible strategy of in-situ constructing all-scale hierarchical nanostructures can also be applied to enhance the performance of other thermoelectric systems.展开更多
基金supported by National Natural Science Foundation of China(NSFC)(grant nos.52063019,51973088,51833004,U20A20128).
文摘The inevitable ion migration that occurs within ionic polycrystalline perovskite film results in inferior longterm stability of perovskite solar cells(PVSCs)that cannot meet the commercial requirements.Here,a novel poly(ionic liquid)named poly-1-vinyl-3-propyltrimethoxysilane imidazolium chloride(PImIL-SiO)is first introduced into perovskite to strengthen grain boundaries(GBs)and construct dual-functional barriers against internal ion migration and external moisture erosion for fabricating highly efficient and stable PVSCs.PImIL-SiO-containing imidazoliumcations and pendant siloxane groups contribute to passivation of bulk defects and anchoring of GBs,which effectively hinders ion migration channels,thus reducing perovskite film phase separation and device hysteresis.Furthermore,the intrinsically hydrophobic PImIL-SiO automatically forms a secondary protective barrier to endow the perovskite film with ultrahigh moisture corrosion resistance through the hydrolyzation reaction of siloxane with the permeated moisture.Consequently,the PImIL-SiO-modified PVSCs achieve a champion power conversion efficiency(PCE)of 22.46%,accompaniedby excellent thermal andhumidity stabilities where the non-encapsulated devices retain 87%of the initial PCE after aging at 85℃for 250 h and>85%of the initial PCE over 1100 h in air with a relative humidity of 50–70%.
基金This work was financially supported by the National Natural Science Foundation of China(NSFC)(grant nos.52063019,51973088,51833004,and U20A20128)the“Double Thousand Plan”Science and Technology Innovation High-end Talent Project of Jiangxi Province(grant no.jxsq2019201107).
文摘The novel triplet–triplet annihilation(TTA)upconversion(UC)field of rubrene(Rub)and dibenzotetraphenylperiflanthene(DBP)sensitized by bulk metal halide perovskite,integrated with copper-2,3,9,10,16,17,23,24-octafluorophthalocyanine(F_(8)CuPc)as cosensitizer,have been investigated in perovskite solar cells(PVSCs)to minimize sub-bandgap photon transmission loss.The firm hydrogen bonding interaction(F…H–N between F_(8)CuPc and MA+),cation-πinteraction(MA+with Rub),and the hydrophobic characteristic of additives enable F_(8)CuPc:Rub:DBP dually-sensitized p-i-n PVSCs based on MAPbI_(3)and Cs_(0.05)(FA_(0.83)MA_(0.17))_(0.95)Pb(Br_(0.17)I_(0.83))_(3)absorbers to attain champion efficiencies of 20.83%and 21.51%,respectively.Furthermore,due to the excellent photochemical and thermal stability of F_(8)CuPc,the corresponding PVSCs can maintain nearly 80%of the original efficiencies exposed to air with 50∼70%relative humidity over 1100 h and N_(2)at 85℃for 300 h.
基金National Natural Science Foundation of China(52272123,52072301)the National Key R&D Program of China(Grant Number:2022YFB3504901)+5 种基金the China-Poland International Collaboration Fund of National Natural Science Foundation of China(No.51961135301)the International CooperationFoundation of Shaanxi Province(2022 KW-34)the Fundamental Research Funds for the Central Universities(No.D5000210722)the Research Fund of State Key Laboratory of Solidification Processing,NPU)(No.2021-TS-08)the Open Fund of State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(No.KFZD202102)the‘111’Project(No.B20028).
文摘SrTiO_(3)-based oxides have been investigated as a promising n-type thermoelectric material at high temperatures;however,the relatively high thermal conductivity results in inferior thermoelectric performance.The lattice thermal conductivity can be significantly reduced by high-entropy engineering via severe lattice distortion.However,high configuration entropy also causes the deterioration of carrier mobility and restrains electron transport resulting in low electrical conductivity.In this work,the low lattice thermal conductivity of 1.7 W/(m·K)at 1073 K and significantly improved electrical conductivity of 112 S/cm from 60 S/cm can be achieved in n-type(Sr_(0.25)Ca_(0.25)Ba_(0.25)La_(0.25))TiO_(3)/Pb@Bi composites ceramics with core-shell grains of all-scale hierarchical microstructure.The effects of the complex microstructure of core-shell grains as well as the precipitated Pb@Bi particles on electrons and phonons transport properties were systematically explored.ZTmax of 0.18 was obtained for the SPS-1200,which was 1.5 times that of pure high-entropy(Ca_(0.2)Sr_(0.2)Ba_(0.2)La_(0.2)Pb_(0.2))TiO_(3)samples prepared by a solid-state method.This improvement in thermoelectric performance contributes to the addition of Bi_(2)O_(3)into the high-entropy(Sr_(0.2)Ca_(0.2)Ba_(0.2)Pb_(0.2)La_(0.2))TiO_(3)matrix resulting in multiphase core-shell grain structure combined with well-dispersed nano-sized metal Pb@Bi precipitates in the matrix.This feasible strategy of in-situ constructing all-scale hierarchical nanostructures can also be applied to enhance the performance of other thermoelectric systems.
