Li Qianrui, Yuan Jinping, Zhao Di, Wang Yige, Li Huanrong
National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering and Technology, Hebei University of Technology, GuangRong Dao 8, Hongqiao District, Tianjin 300130, P. R. China.
Inorg Chem. 2023 Nov 6;62(44):18299-18306. doi: 10.1021/acs.inorgchem.3c03079. Epub 2023 Oct 26.
Zeolite-confined silver nanoclusters (Ag-zeolite) have aroused vast interest due to their remarkable luminescence. The countercations within a zeolite play critical roles in determining the luminescent properties of the resulting Ag-zeolite. We observed, in this work, that introducing Mg enabled the Ag-13X zeolite a stable and bright yellow emission with a high PLQY of 94.6%, the first report on the luminescence enhancement of the Ag-13X zeolite by Mg, to the best of our knowledge. The formation of specific internal electric fields inside 13X and the structural contraction of the zeolite framework due to the high charge density and the small ionic radius of Mg are believed to be responsible for the enhanced stable and bright yellow emission. The stabilization effect of Mg is removed by increasing the heating temperature above 700 °C, which leads to the variation of silver nanoclusters as a result of the framework collapse of the zeolite. The Ag-zeolite synthesized by us, featured with a broad emission band, a high PLQY of 94.6%, and good thermal stability, can be considered a suitable candidate to replace the traditional commercial yellow-emitting phosphor YAG:Ce for light-based applications. This work contributes to a valuable reference for the rational design of silver nanoclusters confined in zeolites with promising new functionalities and stimulates potential applications as novel phosphors for near-ultraviolet light-emitting diodes (NUV-LEDs).
沸石限域银纳米团簇(Ag-沸石)因其显著的发光特性而引起了广泛关注。沸石中的抗衡阳离子在决定所得Ag-沸石的发光性质方面起着关键作用。在这项工作中,我们观察到引入镁能使Ag-13X沸石产生稳定且明亮的黄色发射,其PLQY高达94.6%,据我们所知,这是关于镁增强Ag-13X沸石发光的首次报道。13X内部特定内电场的形成以及由于镁的高电荷密度和小离子半径导致的沸石骨架结构收缩被认为是增强稳定且明亮黄色发射的原因。当加热温度升高到700℃以上时,镁的稳定作用消失,这由于沸石骨架坍塌导致银纳米团簇发生变化。我们合成的Ag-沸石具有宽发射带、94.6%的高PLQY以及良好的热稳定性,可被视为替代传统商用黄色发光荧光粉YAG:Ce用于光基应用的合适候选材料。这项工作为合理设计具有新功能的限域在沸石中的银纳米团簇提供了有价值的参考,并激发了其作为新型荧光粉用于近紫外发光二极管(NUV-LEDs)的潜在应用。