Owing to their unique optical properties and nontoxicity,lead-free halide double perovskite nanocrystals are of interest for widespread applications.Herein,the colloid synthesis and photoluminescenc e property of Ag^(...Owing to their unique optical properties and nontoxicity,lead-free halide double perovskite nanocrystals are of interest for widespread applications.Herein,the colloid synthesis and photoluminescenc e property of Ag^(+)-Eu^(3+)codoped Cs_(2)NaInCl_(6)nanocrystals were investigated.The pe rovskite nanocrystals exhibit a broad warm-white photo luminescence with correlated color temperature(CCT)of 3447 K and color rendering index(CRI)of 90.2,and the means of codoping would improve its optical performance.A fast energy transfer and a long-lived self-trapped excitons state are unveiled by the femtosecond transient absorption spectra.The fast energy transfer from the self-trapped excitons of host nanocrystals to the Eu^(3+)ions is helpful to achieve a broad photoluminescence,and the quantum yield of Cs_(2)NaInCl_(6):0.05Ag^(+)-Eu^(3+)anocrystals can be enha nced to 69.5%.There is a large exciton binding energy and strong electron-phonon interaction in the codoped perovskite nanocrystals.The efficient and excellent air-stable double perovskite nanocrystals would be considered as a single-component phosphor for warm-white lighting.展开更多
Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,...Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer.展开更多
Lead-free halide double perovskites have gathered wide scientific interest since they are environmentally friendly and stable.However,compared to the lead perovskites,their optoelectronic properties are compromised.He...Lead-free halide double perovskites have gathered wide scientific interest since they are environmentally friendly and stable.However,compared to the lead perovskites,their optoelectronic properties are compromised.Herein we report a series of bulk lead-free mixed Bi-In halide double perovskites:Cs2AgBi1-xInxCl6(0<x<1).The Cs2AgBi0.125In0.875Cl6breaks the parity-forbidden transition and retains direct band gap structure,having warm-white light emission,with photoluminescence quantum efficiency(PLQE)of 70.3%,much higher than the PLQE of reported lead perovskite materials.Its exciton self-trapping dynamics is investigated.Meanwhile,the Cs2AgBi0.125In0.875Cl6nanocrystals and Cs2AgBi0.125In0.875Cl6microcrystals can be synthesized by modified hot injection and rapid cooling crystallization,respectively.The size effect of Cs2AgBi0.125In0.875Cl6is studied on the photoluminescence(PL)property.Additionally,the bulk material exhibits excellent stability on exposure to light,humidity and air for more than 3 months.It is a promising candidate as highly efficient warm white-light emitting material for road lighting.展开更多
基金Project supported by the National Natural Science Foundation of China(61805134,11974229,22303044)Fundamental Research Program of Shanxi Province(202203021221121)+3 种基金China Postdoctoral Science Foundation(2022M711898)Natural Science Fo undation of Shandong Province(ZR2023QB135)Postdoctoral Innovation Project of Shandong Province(SDCX-ZG-202201004)Graduate Innovation Project in Shanxi Province(2024KY450)。
文摘Owing to their unique optical properties and nontoxicity,lead-free halide double perovskite nanocrystals are of interest for widespread applications.Herein,the colloid synthesis and photoluminescenc e property of Ag^(+)-Eu^(3+)codoped Cs_(2)NaInCl_(6)nanocrystals were investigated.The pe rovskite nanocrystals exhibit a broad warm-white photo luminescence with correlated color temperature(CCT)of 3447 K and color rendering index(CRI)of 90.2,and the means of codoping would improve its optical performance.A fast energy transfer and a long-lived self-trapped excitons state are unveiled by the femtosecond transient absorption spectra.The fast energy transfer from the self-trapped excitons of host nanocrystals to the Eu^(3+)ions is helpful to achieve a broad photoluminescence,and the quantum yield of Cs_(2)NaInCl_(6):0.05Ag^(+)-Eu^(3+)anocrystals can be enha nced to 69.5%.There is a large exciton binding energy and strong electron-phonon interaction in the codoped perovskite nanocrystals.The efficient and excellent air-stable double perovskite nanocrystals would be considered as a single-component phosphor for warm-white lighting.
基金financially supported by the National Natural Science Foundation of China(22179072,22002070)the Natural Science Foundation of Shandong Province(ZR2021QF006)+3 种基金the Outstanding Youth Science Foundation of Shandong Province(Overseas)(2022HWYQ-006)the Natural Science Foundation of Shandong Province(ZR2020QB059)the Fundamental Research Center of Artificial Photosynthesis(FReCAP)financially supported by the National Natural Science Foundation of China(22088102)the China Postdoctoral Science Foundation(No.2022M711898)。
文摘Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer.
基金supported by the National Natural Science Foundation of China (21533010, 21525315)the National Key Research and Development Program of China (2017YFA0204800)+2 种基金DICP DMTO201601DICP ZZBS201703the Science Challenging Program (JCKY2016212A501)
文摘Lead-free halide double perovskites have gathered wide scientific interest since they are environmentally friendly and stable.However,compared to the lead perovskites,their optoelectronic properties are compromised.Herein we report a series of bulk lead-free mixed Bi-In halide double perovskites:Cs2AgBi1-xInxCl6(0<x<1).The Cs2AgBi0.125In0.875Cl6breaks the parity-forbidden transition and retains direct band gap structure,having warm-white light emission,with photoluminescence quantum efficiency(PLQE)of 70.3%,much higher than the PLQE of reported lead perovskite materials.Its exciton self-trapping dynamics is investigated.Meanwhile,the Cs2AgBi0.125In0.875Cl6nanocrystals and Cs2AgBi0.125In0.875Cl6microcrystals can be synthesized by modified hot injection and rapid cooling crystallization,respectively.The size effect of Cs2AgBi0.125In0.875Cl6is studied on the photoluminescence(PL)property.Additionally,the bulk material exhibits excellent stability on exposure to light,humidity and air for more than 3 months.It is a promising candidate as highly efficient warm white-light emitting material for road lighting.
