高稳定性 CsPbBr3 纳米晶的合成与应用

钙钛矿纳米晶具有优异的光电性能，已在光伏、发光二极管、光催化等领域得到了广泛的关注，也取得了越来越多令人瞩目的成果。尽管如此，钙钛矿材料的稳定性问题仍然突出，其对外部环境的高度敏感性依然是钙钛矿材料商业化应用的最大障碍。因此，解决稳定性问题仍然是现阶段钙钛矿材料研究的重点科学问题之一。本文以提升CsPbBr₃钙钛矿纳米晶的环境稳定性为目标，从惰性基体封装的角度出发，设计了两种不同的钙钛矿纳米晶合成方案，制备了稳定的CsPbBr₃钙钛矿复合材料，并将合成的钙钛矿材料应用于光致发光二极管和水相光催化。

设计了一种气相模板法，原位合成了CsPbBr₃-ZSM-5复合材料，产物具有较高的光致发光量子效率，同时表现出极高的环境稳定性。PbBr₂蒸汽对ZSM-5分子筛孔道的刻蚀作用导致了分子筛结构的崩溃，实现了对纳米晶的有效限域和封装，并提高了钙钛矿材料在恶劣条件下的稳定性。此外，合成的CsPbBr₃-ZSM-5结构具有卤素交换必需的通道，可以调节钙钛矿中的卤素比例，并将大量合成的多色复合材料用于制备白光LED。

开发了一种新型的原位微封装技术，在CsPbBr₃纳米晶表面生长一层很薄的SiO₂网络结构，可以兼顾钙钛矿纳米晶的水相稳定性和电荷传输性能。并说明了钙钛矿纳米晶表面动态平衡状态对后合成钝化的重要意义以及反应体系精细调控对封装效果的影响。将合成的钙钛矿复合材料成功应用于水相降解罗丹明B，说明了其催化活性。

Perovskite nanocrystals have attracted extensive attention in the solar cells, light-emitting diodes, photocatalysis and other fields for their excellent photoelectric properties. Even though remarkable progress has been made in recent years, it is still challengeable to use CsPbBr₃ nanocrystals as commercial materials because of the instability of perovskite materials and the high sensitivity to external environment. Therefore, addressing the stability issue is still one of the key scientific topics in the research of perovskite materials at this stage. In order to improve the environmental stability of CsPbBr₃ nanocrystals, two different synthesis strategies of perovskite nanocrystals were designed to prepare stable CsPbBr₃ perovskite composites from the perspective of inert matrix encapsulation, and the synthesized perovskite materials were applied in photoluminescence diodes and aqueous photocatalysis.

A vapor-phase template method was designed to synthesize CsPbBr₃-ZSM-5 composite in situ, and the product possessed both high PL intensity and high environmental stability. The key chemical reaction between PbBr₂ vapor and Si-O network in ZSM-5 led to the collapse of initial zeolite structure, realizing effective confinement and encapsulation of CsPbBr₃ nanocrystals, and boosting the stability of the nanocrystals under harsh conditions. At the same time, the acquired encapsulation structure possessed the necessary channels for halogen exchange to regulate the halide ratios of CsPbX3-ZSM-5 composites. And the CsPbX3-ZSM-5 composites synthesized on a large scale were applied in white light-emitting diodes (WLEDs).

A novel in-situ post synthetic microencapsulation technology was developed. A thin layer of SiO₂ network was grown on the surface of CsPbBr₃ nanocrystals, which could take into account both the stability and charge transfer performance of perovskite nanocrystals in water. It was explained that the significance of the surface dynamic equilibrium state of perovskite nanocrystals for post synthesis passivation and the influence of fine regulation of the reaction system on the encapsulation effect. The synthesized perovskite composites were used to degrade Rhodamine B in aqueous phase, which showed the catalytic activity.

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