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构建具有两步顺序能量转移的人工光捕获系统用于水中高效光催化的新策略

Novel Strategy of Constructing Artificial Light-Harvesting System with Two-Step Sequential Energy Transfer for Efficient Photocatalysis in Water.

作者信息

Wang Ying, Han Ning, Li Xing-Long, Wang Rong-Zhou, Xing Ling-Bao

机构信息

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

Department of Materials Engineering, KU Leuven, Leuven 3001, Belgium.

出版信息

ACS Appl Mater Interfaces. 2022 Oct 12;14(40):45734-45741. doi: 10.1021/acsami.2c14168. Epub 2022 Sep 27.

Abstract

An efficient artificial light-harvesting system with a two-step sequential energy transfer was fabricated in the aqueous solution based on the host-guest interactions between cyano-substituted -phenylenevinylene derivative (PPTA) and a water-soluble pillar[5]arene (WP5). PPTA-WP5 complex could self-assemble into nanoparticles, and two fluorescent dyes eosin Y (EY) and Nile Red (NIR) are employed as acceptors to realize sequential energy transfer. The PPTA-WP5-EY-NIR system could achieve efficient two-step sequential energy transfer process from PPTA-WP5 to EY and then to NIR (67% for the first step and 66% for the second step). Moreover, to make full use of the harvested energy, the hydrophobic microenvironment in the assembled nanoparticles is used to promote the aerobic cross-dehydrogenative coupling (CDC) reaction in aqueous medium with 88% yield after 12 h of irradiation. To our knowledge, this is the first example of artificial LHS with two-step energy transfer used to catalyze the CDC reaction in aqueous medium. This work directly mimics the function of photosynthesis in nature of converting solar energy into chemical energy in aqueous solution.

摘要

基于氰基取代的对苯撑乙烯衍生物(PPTA)与水溶性柱[5]芳烃(WP5)之间的主客体相互作用,在水溶液中构建了一种具有两步顺序能量转移的高效人工光捕获系统。PPTA-WP5复合物能够自组装成纳米颗粒,并且使用两种荧光染料曙红Y(EY)和尼罗红(NIR)作为受体来实现顺序能量转移。PPTA-WP5-EY-NIR系统能够实现从PPTA-WP5到EY然后到NIR的高效两步顺序能量转移过程(第一步为67%,第二步为66%)。此外,为了充分利用捕获的能量,组装的纳米颗粒中的疏水微环境被用于促进水介质中的需氧交叉脱氢偶联(CDC)反应,在照射12小时后产率为88%。据我们所知,这是首次使用具有两步能量转移的人工光捕获系统在水介质中催化CDC反应的例子。这项工作直接模拟了自然界中光合作用在水溶液中将太阳能转化为化学能的功能。

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