Zhou Hai, Wang Sheng, Wang Haihui, Wang Lin, Chen Jiayi, Jia Guohua, Yang Xuyong
Key Laboratory of Advanced Display and System Applications of Ministry of Education, Shanghai University, 149 Yanchang Road, Shanghai 200072, China.
School of Molecular and Life Sciences, Curtin University, Bentley, WA 6102, Australia.
Nanoscale. 2024 May 23;16(20):10064-10070. doi: 10.1039/d4nr00880d.
The widespread applicability of perovskite nanocrystals (PeNCs) is impeded by their intrinsic instability. A promising solution is utilizing robust chalcogenides as a protective shell to shield the sensitive luminescent cores from the external environment. However, the inferior structural stability and surface lability of PeNCs usually lead to perovskite phase transition during shell growth. Herein, we introduced smaller Zn ions to partially replace Pb ions in perovskites, which reduces the Pb-X bond length and enhances the Pb-X bond energy for inner lattice stabilization. Simultaneously, extra oleylammonium bromide (OAmBr) was added to protect the labile surface of PeNCs by compensating for the detachment of ligands and the loss of surface Br ions. As a result, the dual strategies enable the epitaxial growth of a ZnS shell and significantly enhance the chemical stability of CsZnPbBr/ZnS core/shell PeNCs. After three thermal cycles ranging from 300 to 450 K, the core/shell PeNCs retained 70% of their initial photoluminescence (PL) intensity. In stark contrast, the pristine CsPbBr PeNCs exhibit complete PL quenching after just the first temperature cycle. For practical applications, the green core/shell PeNCs were integrated with commercially available red-emitting phosphors on a blue-emitting InGaN chip to fabricate a white light-emitting diode (WLED), which demonstrates a high luminous efficacy (LE) of 61.3 lm W and nearly constant Commission Internationale de l'Eclairage (CIE) coordinates under varying operating currents.
钙钛矿纳米晶体(PeNCs)的广泛应用受到其固有不稳定性的阻碍。一个有前景的解决方案是利用坚固的硫族化物作为保护壳,以保护敏感的发光核心免受外部环境影响。然而,PeNCs较差的结构稳定性和表面活性通常会导致在壳生长过程中钙钛矿相转变。在此,我们引入较小的锌离子来部分取代钙钛矿中的铅离子,这缩短了Pb-X键长并增强了内晶格稳定的Pb-X键能。同时,添加额外的油胺溴化物(OAmBr)来补偿配体的脱离和表面溴离子的损失,从而保护PeNCs不稳定的表面。结果,这两种策略实现了ZnS壳的外延生长,并显著提高了CsZnPbBr/ZnS核壳PeNCs的化学稳定性。在300至450 K的三个热循环后,核壳PeNCs保留了其初始光致发光(PL)强度的70%。与之形成鲜明对比的是,原始的CsPbBr PeNCs仅在第一个温度循环后就完全发生PL猝灭。对于实际应用,将绿色核壳PeNCs与市售的红色发光磷光体集成在蓝色发光的InGaN芯片上,制造出白光发光二极管(WLED),其在不同工作电流下表现出61.3 lm W的高发光效率(LE)和近乎恒定的国际照明委员会(CIE)坐标。