促进长寿命有机室温磷光的交联聚磷腈纳米球,Journal of the American Chemical Society

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促进长寿命有机室温磷光的交联聚磷腈纳米球
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-03-22 , DOI: 10.1021/jacs.2c02076
Yongfeng Zhang ₁ , Xiaohong Chen ₁ , Jianrong Xu ₁ , Qinglun Zhang ₁ , Liang Gao ₁ , Zhonghao Wang ₁ , Lunjun Qu ₁ , Kaiti Wang ₁ , Youbing Li ₁ , Zhengxu Cai ₂ , Yanli Zhao ₃ , Chaolong Yang _{1,

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Affiliation

由于出色的光学性能和特殊的应用，长寿命有机室温磷光 (RTP) 引发了激烈的探索。由于有机 RTP 中的三重态激子由于其高灵敏度、自旋多重性、不可避免的非辐射衰减和外部猝灭剂而经历了多种弛豫过程，因此通过调制的三重态激子行为提高 RTP 性能具有挑战性。在此，我们报告了交联的聚磷腈纳米球可以有效地促进长寿命的有机 RTP。通过分子工程，多个羰基（C=O）、杂原子（N和P）和重原子（Cl）被引入聚磷腈纳米球，通过重新校准单线态（S_n ) 和三重态 (T _n ) 激子。为了进一步抑制非辐射衰减并避免在环境条件下猝灭，聚磷腈纳米球被聚（乙烯醇）基质包裹，从而同步提高磷光寿命（延长 173 毫秒）、磷光效率（高约 12 倍）、余辉持续时间（超过 20 秒）和余辉绝对亮度（高约 19 倍）与 2,3,6,7,10,11-六羟基苯并苯前体相比。通过测量磷光的发射强度，开发了一种基于纳米球的有效探针，用于可见、定量和快速检测挥发性有机化合物。更重要的是，所得薄膜对苯甲醚检测显示出高选择性和鲁棒性（7.1 × 10 ^–4摩尔 L ^–1 )。这项工作不仅展示了一种提高 RTP 材料效率的方法，而且还为在可行的检测应用中应用 RTP 材料提供了新途径。

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Cross-Linked Polyphosphazene Nanospheres Boosting Long-Lived Organic Room-Temperature Phosphorescence

Long-lived organic room-temperature phosphorescence (RTP) has sparked intense explorations, owing to the outstanding optical performance and exceptional applications. Because triplet excitons in organic RTP experience multifarious relaxation processes resulting from their high sensitivity, spin multiplicity, inevitable nonradiative decay, and external quenchers, boosting RTP performance by the modulated triplet-exciton behavior is challenging. Herein, we report that cross-linked polyphosphazene nanospheres can effectively promote long-lived organic RTP. Through molecular engineering, multiple carbonyl groups (C═O), heteroatoms (N and P), and heavy atoms (Cl) are introduced into the polyphosphazene nanospheres, largely strengthening the spin–orbit coupling constant by recalibrating the electronic configurations between singlet (S_n) and triplet (T_n) excitons. In order to further suppress nonradiative decay and avoid quenching under ambient conditions, polyphosphazene nanospheres are encapsulated with poly(vinyl alcohol) matrix, thus synchronously prompting phosphorescence lifetime (173 ms longer), phosphorescence efficiency (∼12-fold higher), afterglow duration time (more than 20 s), and afterglow absolute luminance (∼19-fold higher) as compared with the 2,3,6,7,10,11-hexahydroxytriphenylene precursor. By measuring the emission intensity of the phosphorescence, an effective probe based on the nanospheres is developed for visible, quantitative, and expeditious detection of volatile organic compounds. More significantly, the obtained films show high selectivity and robustness for anisole detection (7.1 × 10^–4 mol L^–1). This work not only demonstrates a way toward boosting the efficiency of RTP materials but also provides a new avenue to apply RTP materials in feasible detection applications.

更新日期：2022-03-22

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