Luminescent solar concentrators(LSCs)offer a sustainable approach to power generation using fluorescent glasses,yet their green industrialization is impeded by the limited production scale and non-recyclability of emb...Luminescent solar concentrators(LSCs)offer a sustainable approach to power generation using fluorescent glasses,yet their green industrialization is impeded by the limited production scale and non-recyclability of embedded nanocrystals.Here,we introduce a lead-free perovskite derivative ETP_(2)SbCl_(5)(ETP=(C_(6)H_(5))_(3)PC_(2)H_(5))with a reversible transition between powder and glass states.Through molecular dynamics and density functional theory,we elucidate the possible structural distortions of[SbCl_(5)]pyramids and their impact on luminescence.The fabricated LSCs,utilizing such fluorescent glasses with an efficient absorption for<420 nm,achieve the highest power conversion and optical efficiencies of~5.56%and~32.5%,respectively.In addition to self-healing by reheating at~200℃,impressively,it could be mass recycled to phosphor by ethanol or heating treatments,which still maintains nearly initial fluorescent performance and could be repurposed like freshly synthesized samples.This work presents a paradigm for the sustainable use of fluorescent materials and offers a reliable path toward low-carbon globalization.展开更多
Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the r...Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.展开更多
Lead-free halide perovskite materials possess low toxicity,broadband luminescence and robust stability compared with conventional lead-based perovskites,thus holding great promise for eyes-friendly white light LEDs.Ho...Lead-free halide perovskite materials possess low toxicity,broadband luminescence and robust stability compared with conventional lead-based perovskites,thus holding great promise for eyes-friendly white light LEDs.However,the traditionally used preparation methods with a long period and limited product yield have curtailed the commercialization of these materials.Here we introduce a universal hydrochloric acid-assistant powder-to-powder strategy which can accomplish the goals of thermal-,pressure-free,eco-friendliness,short time,low cost and high product yield,simultaneously.The obtained Cs_(2)Na_(0.9)Ag_(0.1)In_(0.95)Bi_(0.05)Cl_(6)microcrystals exhibit bright self-trapped excitons emission with quantum yield of(98.3±3.8)%,which could retain(90.5±1.3)%and(96.8±0.8)%after continuous heating or ultraviolet-irradiation for 1000 h,respectively.The phosphor converted-LED exhibited near-unity conversion efficiency from ultraviolet chip to self-trapped excitons emission at~200 mA.Various ions doping(such as Cs_(2)Na_(0.9)Ag_(0.1)InCl_(6):Ln^(3+))and other derived lead-free perovskite materials(such as Cs_(2)ZrCl_(6)and Cs_(4)MnBi_(2)Cl_(12))with high luminous performance are all realized by our proposed strategy,which has shown excellent availability towards commercialization.展开更多
基金financially supported by the National Natural Science Foundation of China(22275101).
文摘Luminescent solar concentrators(LSCs)offer a sustainable approach to power generation using fluorescent glasses,yet their green industrialization is impeded by the limited production scale and non-recyclability of embedded nanocrystals.Here,we introduce a lead-free perovskite derivative ETP_(2)SbCl_(5)(ETP=(C_(6)H_(5))_(3)PC_(2)H_(5))with a reversible transition between powder and glass states.Through molecular dynamics and density functional theory,we elucidate the possible structural distortions of[SbCl_(5)]pyramids and their impact on luminescence.The fabricated LSCs,utilizing such fluorescent glasses with an efficient absorption for<420 nm,achieve the highest power conversion and optical efficiencies of~5.56%and~32.5%,respectively.In addition to self-healing by reheating at~200℃,impressively,it could be mass recycled to phosphor by ethanol or heating treatments,which still maintains nearly initial fluorescent performance and could be repurposed like freshly synthesized samples.This work presents a paradigm for the sustainable use of fluorescent materials and offers a reliable path toward low-carbon globalization.
基金supported by the National Natural Science Foundation of China(92256202,12261131500,22305129,22371131,52103218)the Fundamental Research Funds for the Central Universities,Nankai University(023-63223021)+3 种基金Tianjin Key Lab for Rare Earth Materials and Applications(ZB19500202)the Outstanding Youth Project of Tianjin Natural Science Foundation(20JCJQJC00130)China Postdoctoral Science Foundation(BX20220157,2022M721698)the 111 Project(B12015,B18030)。
文摘Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.
基金supported by the National Natural Science Foundation of China(22005152,22275101).
文摘Lead-free halide perovskite materials possess low toxicity,broadband luminescence and robust stability compared with conventional lead-based perovskites,thus holding great promise for eyes-friendly white light LEDs.However,the traditionally used preparation methods with a long period and limited product yield have curtailed the commercialization of these materials.Here we introduce a universal hydrochloric acid-assistant powder-to-powder strategy which can accomplish the goals of thermal-,pressure-free,eco-friendliness,short time,low cost and high product yield,simultaneously.The obtained Cs_(2)Na_(0.9)Ag_(0.1)In_(0.95)Bi_(0.05)Cl_(6)microcrystals exhibit bright self-trapped excitons emission with quantum yield of(98.3±3.8)%,which could retain(90.5±1.3)%and(96.8±0.8)%after continuous heating or ultraviolet-irradiation for 1000 h,respectively.The phosphor converted-LED exhibited near-unity conversion efficiency from ultraviolet chip to self-trapped excitons emission at~200 mA.Various ions doping(such as Cs_(2)Na_(0.9)Ag_(0.1)InCl_(6):Ln^(3+))and other derived lead-free perovskite materials(such as Cs_(2)ZrCl_(6)and Cs_(4)MnBi_(2)Cl_(12))with high luminous performance are all realized by our proposed strategy,which has shown excellent availability towards commercialization.
