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室温下双分子质子耦合能量转移的直接证据。

Direct Evidence of Bimolecular Proton-Coupled Energy Transfer at Room Temperature.

作者信息

Rosichini Andrea, Scattolini Giorgio, Hammarström Leif

机构信息

Department of Chemistry, Ångström Laboratory, Uppsala University, Box 523, 75120 Uppsala, Sweden.

出版信息

J Am Chem Soc. 2025 Jul 16;147(28):24181-24185. doi: 10.1021/jacs.5c05126. Epub 2025 Jul 3.

DOI:10.1021/jacs.5c05126
PMID:40607916
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12272677/
Abstract

A new elementary reaction, denoted proton-coupled energy transfer (PCEnT), has been recently reported in a series of donor-acceptor molecules. In this reaction, excited state energy transfer is made possible by a simultaneous transfer of a proton on the energy acceptor. This type of elementary reaction could have, by analogy to proton-coupled electron transfer, an important role in photochemistry and energy transportation of biological systems. In the previously reported case, the reaction is shown to occur intramolecularly in a covalently linked system in a 77 K glass. In this work, we identify a suitable bimolecular system for PCEnT and provide direct evidence for PCEnT in a room temperature solution using fluorescence spectroscopy. Based on these results, we discuss some simple design principles for PCEnT, including some of the current obstacles in designing a successful system.

摘要

最近在一系列供体 - 受体分子中报道了一种新的基元反应,称为质子耦合能量转移(PCEnT)。在该反应中,激发态能量转移通过质子在能量受体上的同时转移而成为可能。类似于质子耦合电子转移,这种类型的基元反应可能在生物系统的光化学和能量传输中发挥重要作用。在先前报道的案例中,该反应在77K玻璃中的共价连接系统中发生分子内反应。在这项工作中,我们确定了一种适用于PCEnT的双分子系统,并使用荧光光谱法在室温溶液中为PCEnT提供了直接证据。基于这些结果,我们讨论了PCEnT的一些简单设计原则,包括设计成功系统时当前面临的一些障碍。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/68f402e6116d/ja5c05126_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/97b4ff3e8998/ja5c05126_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/e896cbcc17e3/ja5c05126_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/68f402e6116d/ja5c05126_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/97b4ff3e8998/ja5c05126_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/e896cbcc17e3/ja5c05126_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4216/12272677/68f402e6116d/ja5c05126_0003.jpg

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本文引用的文献

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Evidence for Competing Proton-Coupled Reaction Pathways of Molecular Triads in a Low-Polarity Solvent.低极性溶剂中分子三元组竞争质子耦合反应途径的证据。
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Theory for proton-coupled energy transfer.质子耦合能量转移理论。
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