无机CsPbX_(3)钙钛矿材料由于其优异的光电性能、较宽的可调带隙及简单的制备工艺而得到广泛关注。溶液制备无机CsPbX_(3)钙钛矿结晶速率过快,结晶质量不高,所获得的CsPbX_(3)薄膜体相和表面存在大量的缺陷,严重影响了CsPbX_(3)钙钛矿...无机CsPbX_(3)钙钛矿材料由于其优异的光电性能、较宽的可调带隙及简单的制备工艺而得到广泛关注。溶液制备无机CsPbX_(3)钙钛矿结晶速率过快,结晶质量不高,所获得的CsPbX_(3)薄膜体相和表面存在大量的缺陷,严重影响了CsPbX_(3)钙钛矿太阳电池(perovskite solar cells,PSCs)的效率和稳定性,因此需要调控CsPbX_(3)薄膜的结晶过程,钝化其缺陷,以便获得高质量的钙钛矿薄膜和高效、稳定的无机CsPbX_(3)PSCs。近年来,前驱体工程已被证明是获得高质量钙钛矿薄膜的有效策略。该文对无机CsPbX_(3)钙钛矿晶体结构、光电性能、制备方法及存在问题等方面进行概述,总结并讨论了基于前驱体工程制备高质量无机CsPbX_(3)钙钛矿薄膜的4种主要方法,包括组分优化、添加剂策略、中间相调控、异质结构筑。其中,组分优化能够有效调控结晶速率和结晶路径;添加剂策略实现对不同类型缺陷的钝化;中间相调控是获得优良的表面形貌和高结晶度钙钛矿薄膜的关键策略;异质结构筑是抑制不利非辐射复合,提高钙钛矿稳定性的有效策略。最后,对无机CsPbX_(3)PSCs研究的发展趋势进行了展望,在未来应该深入探索CsPbX_(3)钙钛矿薄膜结晶机理和缺陷钝化物理机制,以制备高质量钙钛矿薄膜,同时应致力于大面积器件和叠层电池的制备和开发,以实现更高的光电转换效率和商业化应用。展开更多
Perovskite has received extensive attention due to its excellent properties, just like photoelectric, while the instability has always troubled us to the wide application of perovskite materials. Herein, we proposed t...Perovskite has received extensive attention due to its excellent properties, just like photoelectric, while the instability has always troubled us to the wide application of perovskite materials. Herein, we proposed to use SiO_(2)and POE to encapsulate perovskite nanocrystals(PNCs). In this work, we have successfully prepared a series of perovskite composite materials and films with different concentration ratios.Due to the protection of POE, the luminous intensity of CsPbBr_(3)@POE composite film remained above 90% after stayed in the water for 42 days. The lead concentration of CsPbBr_(3)@POE composite film was 0.8 μg/m L after 48 h of immersing in deionized water. Namely, packaging PNCs in POE could effectively prevent Pb from overflowing reduce Pb pollution. Besides, the composite films showed a wide colour gamut with 117% of NTSC colour gamut, which shows that this composite material has a development prospect in the WLED field.展开更多
All-inorganic perovskites are rapidly emerging as novel optoelectronic functional materials owing to their flu-orescence properties.However,the stability of these materials has always been the biggest challenge for th...All-inorganic perovskites are rapidly emerging as novel optoelectronic functional materials owing to their flu-orescence properties.However,the stability of these materials has always been the biggest challenge for their applications in photoelectric devices.Therefore,this study focuses on developing phosphor-aluminosilicate-based CsPbX_(3)(X=Cl,Br,and I)glass with a low reaction temperature by adding CsCO_(3),PbX_(2),and NaX to the raw materials in order to improve the stabilities.The glass network intermediates of SiO_(2) and Al_(2)O_(3) doping in the raw material enhanced the stability of the pure phosphate glass network structure and devitrification while decreas-ing the melting temperature.Full chromatographic CsPbX 3 quantum dots(QDs)encapsulated in phosphate-based glass were found to increase the fluorescence properties and quantum efficiency(>59%).Notably,the high water stability of CsPbX_(3) QDs glasses,with the maintenance of 90% luminous intensity,emerged when soaked in water.In addition,the excellent thermal stability and anti-ion exchange properties of the CsPbX_(3) QDs glasses were re-vealed.Benefiting from the above,multicolor light-emitting diode(LED)devices were assembled with a mixture of phosphors of CsPbX_(3) QDs glasses and commercial red-emission K 2 SiF 6:Mn 4+phosphor spread on an InGaN chip,demonstrating bright light with superior luminous properties.Phosphor-aluminosilicate-based CsPbX_(3) QDs glass with high stability and low formation temperature would provide new methods for applications in lighting and displays.展开更多
Rapid halide anion exchange easily occurring in metal-halide perovskite nanoparticles(NPs)makes it nearly impossible to create a single three-dimensional(3D)CsPbX_(3)(X=Cl,Br,I)NP that simultaneously comprises two sep...Rapid halide anion exchange easily occurring in metal-halide perovskite nanoparticles(NPs)makes it nearly impossible to create a single three-dimensional(3D)CsPbX_(3)(X=Cl,Br,I)NP that simultaneously comprises two separate perovskite components.To circumvent this problem,we first propose a Ni^(2+)-mediated halide anion-exchange strategy in zero-dimensional(0D)Ni^(2+)-doped Cs_(4)PbBr_(6)(Cs_(4)PbBr_(6):Ni)perovskites to achieve ultra-stable 3D CsPbX_(3)NPs with two coexisting different perovskite individuals of CsPbCl_(3)and/or CsPbBr_(3).By combining the experimental results with first-principles calculations,we confirm that the completely isolated[PbBr_(6)]4−octahedra in 0D Cs_(4)PbBr_(6):Ni NPs can restrict rapid halide anion exchange and the anion diffusion preferentially proceeds in the proximity of substitutional NiPb centers,namely[NiBr_(6)]4−octahedra in a meta-stable state,rather than in the 0D Cs_(4)PbBr_(6)and residual 3D CsPbBr_(3)regions,thereby delivering intrinsic dual-band excitonic luminescence from a single 3D CsPbX_(3)NP with a more stable and efficient CsPbCl_(3)component as compared to its counterparts synthesized using conventional methods.These new insights regarding the precise control of halide anion exchange enable the preparation of a new type of high-efficiency perovskite materials with suppressed anion interdiffusion for prospective optoelectronic devices.展开更多
All-inorganic cesium lead halide perovskite nanocrystals(CsPbX_(3),X=Cl,Br,I)have attracted considerable scientific and technological interest due to their precise bandgap tunability,high color purity and efficient lu...All-inorganic cesium lead halide perovskite nanocrystals(CsPbX_(3),X=Cl,Br,I)have attracted considerable scientific and technological interest due to their precise bandgap tunability,high color purity and efficient luminescence.Nevertheless,their poor stability in harsh conditions such as moisture,ultraviolet(UV)light irradiation and high temperature,is a major obstacle for their further commercial applications.Herein,by simply using a new type of precursor,namely“HPbX_(3)”(X=Cl,Br,I),we can achieve the coordination equilibrium for Pb precursors during reaction and obtain high-quality perovskite nanocrystals with tremendously enhanced luminous efficiency and chemical stability based on hot-injection method.The prepared a-CsPbb nanocrystals exhibit an extremely high photoluminescence quantum yield of 96%and keep stable in air for more than two months without any post-synthesis treatment.Moreover,stability evaluations under UV light irradiation,water or thermal impact are also performed and the results show substantially improved stability of these nanocrystals as compared with the samples prepared using traditional Pbl_(2) as precursor.Through temperature-dependent(10-300 K)steady and transient spectral analysis combined with compositional measurements,it is revealed that the lower structural defect density,which is guaranteed by abundant halogen when using HPbX3 as precursor,is the most important reason for such performance enhancement.展开更多
文摘无机CsPbX_(3)钙钛矿材料由于其优异的光电性能、较宽的可调带隙及简单的制备工艺而得到广泛关注。溶液制备无机CsPbX_(3)钙钛矿结晶速率过快,结晶质量不高,所获得的CsPbX_(3)薄膜体相和表面存在大量的缺陷,严重影响了CsPbX_(3)钙钛矿太阳电池(perovskite solar cells,PSCs)的效率和稳定性,因此需要调控CsPbX_(3)薄膜的结晶过程,钝化其缺陷,以便获得高质量的钙钛矿薄膜和高效、稳定的无机CsPbX_(3)PSCs。近年来,前驱体工程已被证明是获得高质量钙钛矿薄膜的有效策略。该文对无机CsPbX_(3)钙钛矿晶体结构、光电性能、制备方法及存在问题等方面进行概述,总结并讨论了基于前驱体工程制备高质量无机CsPbX_(3)钙钛矿薄膜的4种主要方法,包括组分优化、添加剂策略、中间相调控、异质结构筑。其中,组分优化能够有效调控结晶速率和结晶路径;添加剂策略实现对不同类型缺陷的钝化;中间相调控是获得优良的表面形貌和高结晶度钙钛矿薄膜的关键策略;异质结构筑是抑制不利非辐射复合,提高钙钛矿稳定性的有效策略。最后,对无机CsPbX_(3)PSCs研究的发展趋势进行了展望,在未来应该深入探索CsPbX_(3)钙钛矿薄膜结晶机理和缺陷钝化物理机制,以制备高质量钙钛矿薄膜,同时应致力于大面积器件和叠层电池的制备和开发,以实现更高的光电转换效率和商业化应用。
基金supported by the National Natural Science Foundation of China(51872207,52072271)。
文摘Perovskite has received extensive attention due to its excellent properties, just like photoelectric, while the instability has always troubled us to the wide application of perovskite materials. Herein, we proposed to use SiO_(2)and POE to encapsulate perovskite nanocrystals(PNCs). In this work, we have successfully prepared a series of perovskite composite materials and films with different concentration ratios.Due to the protection of POE, the luminous intensity of CsPbBr_(3)@POE composite film remained above 90% after stayed in the water for 42 days. The lead concentration of CsPbBr_(3)@POE composite film was 0.8 μg/m L after 48 h of immersing in deionized water. Namely, packaging PNCs in POE could effectively prevent Pb from overflowing reduce Pb pollution. Besides, the composite films showed a wide colour gamut with 117% of NTSC colour gamut, which shows that this composite material has a development prospect in the WLED field.
基金This work was supported in part by the China Postdoctoral Science Foundation(No.2022M711438)'the Natural Science Foundation of Shandong Province(ZR2020ME045 and ZR2020ME046)'the“New Universities 20”Foundation of Jinan(Grant No.2021GXRC099).
文摘All-inorganic perovskites are rapidly emerging as novel optoelectronic functional materials owing to their flu-orescence properties.However,the stability of these materials has always been the biggest challenge for their applications in photoelectric devices.Therefore,this study focuses on developing phosphor-aluminosilicate-based CsPbX_(3)(X=Cl,Br,and I)glass with a low reaction temperature by adding CsCO_(3),PbX_(2),and NaX to the raw materials in order to improve the stabilities.The glass network intermediates of SiO_(2) and Al_(2)O_(3) doping in the raw material enhanced the stability of the pure phosphate glass network structure and devitrification while decreas-ing the melting temperature.Full chromatographic CsPbX 3 quantum dots(QDs)encapsulated in phosphate-based glass were found to increase the fluorescence properties and quantum efficiency(>59%).Notably,the high water stability of CsPbX_(3) QDs glasses,with the maintenance of 90% luminous intensity,emerged when soaked in water.In addition,the excellent thermal stability and anti-ion exchange properties of the CsPbX_(3) QDs glasses were re-vealed.Benefiting from the above,multicolor light-emitting diode(LED)devices were assembled with a mixture of phosphors of CsPbX_(3) QDs glasses and commercial red-emission K 2 SiF 6:Mn 4+phosphor spread on an InGaN chip,demonstrating bright light with superior luminous properties.Phosphor-aluminosilicate-based CsPbX_(3) QDs glass with high stability and low formation temperature would provide new methods for applications in lighting and displays.
基金supported by the National Natural Science Foundation of China(61904023 and 11974063)the Natural Science Foundation of Chongqing(cstc2019jcyj-bsh X0078)。
基金supported by the Fund of Fujian Science&Technology Innovation Laboratory for Optoelectronic Information(grant nos.2020ZZ114 and 2022ZZ204)the Key Research Program of Frontier Science CAS(grant no.QYZDY-SSW-SLH025)+1 种基金the National Natural Science Foundation of China(grant nos.21731006 and 21871256)the Fund of Advanced Energy Science and Technology Guangdong Laboratory(grant no.DJLTN0200/DJLTN0240).
文摘Rapid halide anion exchange easily occurring in metal-halide perovskite nanoparticles(NPs)makes it nearly impossible to create a single three-dimensional(3D)CsPbX_(3)(X=Cl,Br,I)NP that simultaneously comprises two separate perovskite components.To circumvent this problem,we first propose a Ni^(2+)-mediated halide anion-exchange strategy in zero-dimensional(0D)Ni^(2+)-doped Cs_(4)PbBr_(6)(Cs_(4)PbBr_(6):Ni)perovskites to achieve ultra-stable 3D CsPbX_(3)NPs with two coexisting different perovskite individuals of CsPbCl_(3)and/or CsPbBr_(3).By combining the experimental results with first-principles calculations,we confirm that the completely isolated[PbBr_(6)]4−octahedra in 0D Cs_(4)PbBr_(6):Ni NPs can restrict rapid halide anion exchange and the anion diffusion preferentially proceeds in the proximity of substitutional NiPb centers,namely[NiBr_(6)]4−octahedra in a meta-stable state,rather than in the 0D Cs_(4)PbBr_(6)and residual 3D CsPbBr_(3)regions,thereby delivering intrinsic dual-band excitonic luminescence from a single 3D CsPbX_(3)NP with a more stable and efficient CsPbCl_(3)component as compared to its counterparts synthesized using conventional methods.These new insights regarding the precise control of halide anion exchange enable the preparation of a new type of high-efficiency perovskite materials with suppressed anion interdiffusion for prospective optoelectronic devices.
基金supported by the Priority Research Project of Xiamen(No.3502Z20191015)。
文摘All-inorganic cesium lead halide perovskite nanocrystals(CsPbX_(3),X=Cl,Br,I)have attracted considerable scientific and technological interest due to their precise bandgap tunability,high color purity and efficient luminescence.Nevertheless,their poor stability in harsh conditions such as moisture,ultraviolet(UV)light irradiation and high temperature,is a major obstacle for their further commercial applications.Herein,by simply using a new type of precursor,namely“HPbX_(3)”(X=Cl,Br,I),we can achieve the coordination equilibrium for Pb precursors during reaction and obtain high-quality perovskite nanocrystals with tremendously enhanced luminous efficiency and chemical stability based on hot-injection method.The prepared a-CsPbb nanocrystals exhibit an extremely high photoluminescence quantum yield of 96%and keep stable in air for more than two months without any post-synthesis treatment.Moreover,stability evaluations under UV light irradiation,water or thermal impact are also performed and the results show substantially improved stability of these nanocrystals as compared with the samples prepared using traditional Pbl_(2) as precursor.Through temperature-dependent(10-300 K)steady and transient spectral analysis combined with compositional measurements,it is revealed that the lower structural defect density,which is guaranteed by abundant halogen when using HPbX3 as precursor,is the most important reason for such performance enhancement.
