新一代白光LED用全光谱CsPbX3(X=Cl、Br、I）钙钛矿量子点微晶玻璃的研究

All-inorganic cesium lead halide perovskites CsPbX3 quantum dots (QDs) exhibit excellent luminescent properties, such as entire visible spectral region, narrow emission band, high quantum efficiency, and color tunability. Hence, perovskites CsPbX3 nanocrystals are promising candidates for next-generation innovative lighting, but their commercialization is hindered by their relatively poor chemical and thermal stability. The inorganic CsPbX3 nanacrystals will be synthesized by hot injection and modified by choosing different ligands. To improve chemical and thermal stability, sodium borosilicate glass doped the CsPbX3 QDs will be prepared by the sol-gel method and glass ceramics containing the CsPbX3 QDs will be fabricated by low-temperature co-sintering method. The effects of the species of added precursors, glass compositions, sintering temperature and sintering atmosphere on the preparation of glass are explored. The formation mechanisms of monodisperse, high concentration of CsPbX3 QDs uniformly dispersed in the glass are discussed. Meanwhile, the effects of ligands, glass composition and preparation process on the emission wavelength, PL intensity, lifetime, quantum efficiency are mainly evaluated. The relationship of the microstructure and optical properties is established and the compatibility of glass and CsPbX3 QDs is improved. The W-LED optical performances excited by the blue-emitting chip are studied. Finally, the glass ceramics doped CsPbX3 QDs with the entire visible spectral region, narrow emission band and color tunability are obtained .

全无机CsPbX3钙钛矿量子点由于具有全光谱、窄发射带、高量子产率，颜色可调等优异的光学性质，在新一代照明器件中具有重要的应用，但相对差的化学和热稳定性将阻碍其应用。因此，本项目用热注入法合成CsPbX3纳米晶，并进行修饰，用溶胶凝胶法制备含有CsPbX3量子点的钠硼硅玻璃，用低温共烧法熔制含有CsPbX3量子点微晶玻璃，以提高其化学稳定性和热稳定性。摸索先驱体种类、玻璃组成、烧结温度、烧结气氛等因素对制备CsPbX3微晶玻璃的影响，探讨单分散、高浓度、均匀掺杂 CsPbX3纳米晶在玻璃中的形成机理，重点评价量子点表面包覆、玻璃组分及制备工艺对微晶玻璃发光波长、强度、寿命、量子产率的影响，建立玻璃微结构与发光性能的关系，改进玻璃与CsPbX3量子点的相容性，研究CsPbX3量子点微晶玻璃在蓝光芯片激发下白光LED的发光性能，获得全光谱、窄发射带、颜色可调CsPbX3钙钛矿量子点微晶玻璃。

CsPbX3钙钛矿量子点具有发射光谱可调，带宽窄，量子产率高，色域宽等特性，在太阳能电池、发光二极管(LED)、激光器、光催化等领域得到广泛关注，然而 CsPbX3钙钛矿量子点稳定性差，限制了其应用。本项目以探索高稳定性、高量子产率、CsPbX3钙钛矿量子点玻璃为研究目标，开展了系列的研究，率先采用熔融热处理及原位析晶方法成功地制备了绿色CsPbBr3量子点玻璃，引领了超稳定、高性能钙钛矿量子玻璃的研究；随后成功制备了CsPb2Br5量子点玻璃；通过调节卤素Br、I比，在磷硅酸盐玻璃中成功制备了系列CsPbBrxI3-x纳米晶玻璃，实现了(523~693 nm)绿光到红光连续可调。将CsPbBrxI3-x玻璃与商业InGaN蓝色芯片耦合可分别制造绿色LED、红色LED和白色LED 。白光LED器件CIE颜色坐标为(0.3299, 0.3322)，非常接近标准白色 (0.33, 0.33)，光效102.4lm/W，色温5176，显指74。通过调节Cl、Br、I比例及基础玻璃组分成功的在硼硅酸盐玻璃中制造了CsPbX3系列纳米晶玻璃，不仅实现了全光谱可调，还实现了全光谱上转换发光，并且首先在玻璃中实现红、蓝、绿上转换放大的自发辐射，开辟了钙钛矿量子点玻璃激光器研究新时代。.我们还采用正硅酸乙酯、正硅酸甲酯等为先驱体成功制备了高稳定性发光量子点，正硅酸乙酯不仅提高了钙钛矿量子点的化学高稳定性，还可以调节CsPb2Br5和CsPbBr3相变。.通过A位掺杂（K+、Rb+）和B位掺杂（稀土、过渡、其它金属离子）可以适当降低铅含量，调节能带结构，提高量子效率等光电性能。.项目研究发表相关论文33篇，申请专利6项，培养硕士研究生 10名。