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Mechanosynthesis of polymer-stabilized lead bromide perovskites: insight into the formation and phase conversion of nanoparticles
Nano Research ( IF 9.5 ) Pub Date : 2020-11-02 , DOI: 10.1007/s12274-020-3152-7
Guocan Jiang , Onur Erdem , René Hübner , Maximilian Georgi , Wei Wei , Xuelin Fan , Jin Wang , Hilmi Volkan Demir , Nikolai Gaponik

The application of polymers to replace oleylamine (OLA) and oleic acid (OA) as ligands for perovskite nanocrystals is an effective strategy to improve their stability and durability especially for the solution-based processing. Herein, we report a mechanosynthesis of lead bromide perovskite nanoparticles (NPs) stabilized by partially hydrolyzed poly(methyl methacrylate) (h-PMMA) and high-molecular-weight highly-branched poly(ethylenimine) (PEI-25K). The as-synthesized NP solutions exhibited green emission centered at 516 nm, possessing a narrow full-width at half-maximum of 17 nm and as high photoluminescence quantum yield (PL QY) as 85%, while showing excellent durability and resistance to polar solvents, e.g., methanol. The colloids of polymer-stabilized NPs were directly processable to form stable and strongly-emitting thin films and solids, making them attractive as gain media. Furthermore, the roles of h-PMMA and PEI-25K in the grinding process were studied in depth. The h-PMMA can form micelles in the grinding solvent of dichloromethane to act as size-regulating templates for the growth of NPs. The PEI-25K with large amounts of amino groups induced significant enrichment of PbBr2 in the reaction mixture, which in turn caused the formation of CsPb2Br5-mPbBr2 and CsPbBr3-Cs4PbBr6-nCsBr NPs. The presence of CsPbBr3-Cs4PbBr6-nCsBr NPs was responsible for the high PL QY, as the Cs4PbBr6 phase with a wide energy bandgap can passivate the surface defects of the CsPbBr3 phase. This work describes a direct and facile mechanosynthesis of polymer-coordinated perovskite NPs and promotes in-depth understanding of the formation and phase conversion for perovskite NPs in the grinding process.



中文翻译:

聚合物稳定的溴化铅钙钛矿的机械合成:洞察纳米颗粒的形成和相变

应用聚合物代替油酸胺(OLA)和油酸(OA)作为钙钛矿纳米晶体的配体是一种提高其稳定性和耐久性的有效策略,尤其是对于基于溶液的工艺。在这里,我们报告了由部分水解的聚甲基丙烯酸甲酯(h-PMMA)和高分子量高支化聚(乙烯亚胺)(PEI-25K)稳定的溴化钙钛矿铅纳米颗粒(NPs)的机械合成。合成后的NP溶液显示出以516 nm为中心的绿色发射,半峰全宽为17 nm,具有窄的全宽度,并且具有高达85%的高光致发光量子产率(PL QY),同时具有出色的耐久性和对极性溶剂的耐受性,例如甲醇。聚合物稳定的NP的胶体可直接加工形成稳定且强发射的薄膜和固体,使他们成为吸引媒体的吸引力。此外,深入研究了h-PMMA和PEI-25K在研磨过程中的作用。h-PMMA可以在二氯甲烷的研磨溶剂中形成胶束,充当NPs生长的尺寸调节模板。带有大量氨基的PEI-25K引起PbBr的显着富集2在反应混合物中,进而导致形成CsPb 2 Br 5 - m PbBr 2和CsPbBr 3 -Cs 4 PbBr 6 - n CsBr NPs。CsPbBr的存在3 -Cs 4 PbBr 6 - ñ溴化铯的NP是负责高PL QY,作为CS 4 PbBr 6相具有宽能带隙可钝化CsPbBr的表面缺陷3相。这项工作描述了聚合物配位的钙钛矿NP的直接而简单的机械合成,并促进了对研磨过程中钙钛矿NP的形成和相变的深入了解。

更新日期:2021-01-10
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