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基于磷光级联能量转移的可调谐多色超分子组装体用于光催化有机转化和防伪

Tunable multicolor supramolecular assemblies based on phosphorescence cascade energy transfer for photocatalytic organic conversion and anti-counterfeiting.

作者信息

Zhu Rong-Xin, Ge Hui-Cong, Niu Kai-Kai, Liu Hui, Dong Ruizhi, Yu Shengsheng, Xing Ling-Bao

机构信息

School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255000, PR China.

School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255000, PR China.

出版信息

J Colloid Interface Sci. 2024 Dec;675:893-903. doi: 10.1016/j.jcis.2024.07.062. Epub 2024 Jul 8.

Abstract

Making full use of the captured energy by phosphorescence light-harvesting systems (PLHSs) and the tunable photoluminescence in energy transfer process to realize the multiple applications is still the challenge of PLHSs research. In this study, we have successfully constructed a highly effective PLHS with tunable multicolor luminescence and efficient conversion of photosensitizer types, which can further be used in photocatalytic organic conversion, information anti-counterfeiting and storage. The supramolecular polymer of BDBP-CB[8], which is generated by cucurbit[8]uril (CB[8]) and 4-(4-bromophenyl)-pyridine derivative (BDBP), realizes a phosphorescence emission and a change in luminescence color. Notably, white light emission was achieved and the logic gate systems were constructed utilizing the application of adjustable luminescence color. More interestingly, PLHS can be constructed by employing BDBP-CB[8] as energy donors, Sulforhodamine 101 (SR101) and Cyanine5 (Cy5) as energy acceptors, which results in a remarkably tunable multicolor photoluminescence to achieve the information storage. Furthermore, we have also found that BDBP-CB[8] can serve as type II photosensitizer for the effective production of singlet oxygen (O) during the photooxidation process of styrene in aqueous environments, attaining a remarkable output rate reaching as high as 89 %. Particularly, compared with O produced by type II photosensitizer BDBP-CB[8], the construction of PLHS can effectively convert type II photosensitizer to type I photosensitizer and efficiently generate superoxide anion radical (O), which can be used for photocatalytic cross-dehydrogenative coupling (CDC) reaction in the aqueous solution with a yield of 90 %. Thus, we have created a PLHS that not only achieves tunable multicolor emission for information anti-counterfeiting and storage, but also realizes the conversion of reactive oxygen species (ROS) for different types photocatalytic oxidation reactions.

摘要

充分利用磷光光捕获系统(PLHSs)捕获的能量以及能量转移过程中可调谐的光致发光来实现多种应用,仍然是PLHSs研究面临的挑战。在本研究中,我们成功构建了一种具有可调谐多色发光和高效光敏剂类型转换的高效PLHS,其可进一步用于光催化有机转化、信息防伪和存储。由葫芦[8]脲(CB[8])和4-(4-溴苯基)-吡啶衍生物(BDBP)生成的BDBP-CB[8]超分子聚合物实现了磷光发射和发光颜色变化。值得注意的是,实现了白光发射,并利用可调发光颜色构建了逻辑门系统。更有趣的是,以BDBP-CB[8]作为能量供体、磺基罗丹明101(SR101)和花菁5(Cy5)作为能量受体可构建PLHS,从而产生显著可调谐的多色光致发光以实现信息存储。此外,我们还发现BDBP-CB[8]可作为II型光敏剂,在水环境中苯乙烯的光氧化过程中有效产生活性单线态氧(O),产率高达89%。特别地,与II型光敏剂BDBP-CB[8]产生的O相比,PLHS的构建可有效将II型光敏剂转化为I型光敏剂并高效产生超氧阴离子自由基(O),其可用于水溶液中的光催化交叉脱氢偶联(CDC)反应,产率为90%。因此,我们创建了一种PLHS,其不仅实现了用于信息防伪和存储的可调谐多色发射,还实现了用于不同类型光催化氧化反应的活性氧(ROS)转换。

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