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Bidentate oxalate ion enhancing water-resistant stability and exciton recombination behavior of blue CsPb(Br/Cl)3 quantum dots
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-08-29 , DOI: 10.1016/j.cej.2023.145732
Le Ma , Xiansheng Li , Xuehan Chen , Jingyu Li , Pengfei Liu , Changting Wei , Qingshan Ma , Leimeng Xu , Wenhua Zhang , Jizhong Song

Mixed halide CsPb(Br/Cl)3 quantum dots (QDs) exhibit fine tunable blue light and narrow photoluminescence full-width at half-maximum (FWHM), which has attracted significant attention as a promising candidate to realize a new generation of blue light technology. However, the introduction of Cl makes it very easy to be eroded by water in the environment, which will lead to deep-level defects and degrade the luminescence and stability of QDs. Here, we propose to introduce tetra-n-octylammonium oxalate (TOAOxa) to improve the water-resistance stability and exciton recombination of CsPb(Br/Cl)3 QDs and QD based light-emitting diodes (QLEDs). The oxalate ion (Oxa2−) of TOAOxa could form strong interaction with undercoordinated Pb2+ on CsPb(Br/Cl)3 QD surface, which was confirmed by FTIR and XPS analysis. Oxa2− passivated QDs (Oxa-QDs) exhibited improved photoluminescence quantum yield (PLQY) and enhanced water-resistance stability compared to pristine QDs. For example, after soaking in water–acetone co-solvent for 1 h, Oxa-QDs can maintain the initial cubic morphology and 43.9% of initial PL intensity, while the morphology and luminescence of pristine QDs are almost damaged. Based on the above concept, the Oxa-QD-based QLED presented a maximum external quantum efficiency (EQE) of 4.0%, and operational lifetime (T50) of 84 s, which was a 5-fold enhancement in EQE, and 7-fold enhancement in stability compared to pristine QLED, respectively. Besides, the Oxa-QD-based QLED exhibits better stability in high-humidity air. To sum up, the Oxa2− passivation strategy has significantly improved the efficiency and water-resistant stability of QDs and devices and would rapidly promote the development of blue-emitting QDs.



中文翻译:

双齿草酸根离子增强蓝色CsPb(Br/Cl)3量子点的耐水稳定性和激子复合行为

混合卤化物CsPb(Br/Cl) 3量子点(QD)表现出精细可调的蓝光和窄光致发光半峰全宽(FWHM),作为实现新一代蓝光的有希望的候选者而受到广泛关注技术。然而, Cl−的引入使其很容易被环境中的水侵蚀,从而导致深能级缺陷,降低量子点的发光和稳定性。在这里,我们建议引入四正辛基草酸铵(TOAOxa)来提高CsPb(Br/Cl) 3 QD和基于QD的发光二极管(QLED)的耐水稳定性和激子复合。草酸根离子 (Oxa 2−TOAOxa ) 可以与CsPb(Br/Cl) 3 QD 表面上的欠配位 Pb 2+形成强相互作用,这一点通过 FTIR 和 XPS 分析得到证实。与原始量子点相比, Oxa 2−钝化量子点(Oxa-QD)表现出更高的光致发光量子产率(PLQY)和增强的耐水稳定性。例如,在水-丙酮共溶剂中浸泡1小时后,Oxa-QDs可以保持初始的立方形貌和初始PL强度的43.9%,而原始QDs的形貌和发光几乎被破坏。基于上述概念,基于Oxa-QD的QLED呈现出4.0%的最大外量子效率(EQE)和工作寿命(T 50) 84 秒,与原始 QLED 相比,EQE 提高了 5 倍,稳定性提高了 7 倍。此外,基于Oxa-QD的QLED在高湿度空气中表现出更好的稳定性。综上所述,Oxa 2−钝化策略显着提高了量子点和器件的效率和耐水稳定性,将迅速推动蓝光量子点的发展。

更新日期:2023-08-30
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