Fluorescence Lifetime Imaging Microscopy (FLIM) as a Tool to Understand Chemical Reactions and Catalysis

Suzanne, Blum, Pia, Lopez
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Abstract

Fluorescence lifetime imaging microscopy (FLIM) is an emerging tool to characterize ongoing chemical reactions in synthetic chemistry and catalysis. Initially applied to biological systems, FLIM now reveals spatially resolved chemical reaction species and system-wide physiochemical changes that accompany ongoing reactions. FLIM combines the advantage of environmental sensitivity with high signal sensitivity (as sensitive as single molecules) and has the key ability to operate under synthetic conditions (e.g., high concentrations of reagents, in organic solvents, under ambient temperature and pressure, in opaque mixtures, and in multiphasic systems). Chemical reactions inherently induce changes in the reaction medium, neighboring compounds, surface compositions, and/or the bonding structure of the compounds involved, resulting in environmental changes. The FLIM methods recently developed harness and interpret these changes in ways that lead to characterizing compounds and enhancing mechanistic understanding. Here, current advantages and limitations of FLIM method are considered, common factors influencing fluorescence lifetime in chemical systems are discussed in a tutorial format, and seven research case studies are strategically analyzed—chosen to highlight how FLIM provided complementary information to understand chemical reaction mechanisms, intermediates, product distributions, partitioning, roles of reagents, and catalyst behaviors. These data and insights obtained from FLIM assist the rational design and optimization of synthetic and catalytic methods.
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荧光寿命成像显微镜 (FLIM) 作为了解化学反应和催化作用的工具
荧光寿命成像显微镜(FLIM)是表征合成化学和催化中正在进行的化学反应的一种新兴工具。荧光寿命成像显微镜最初应用于生物系统,现在可揭示空间分辨的化学反应物种以及伴随正在进行的反应而发生的全系统生理化学变化。FLIM 结合了环境灵敏度和高信号灵敏度(与单分子一样灵敏)的优势,并且具有在合成条件下(如高浓度试剂、有机溶剂、环境温度和压力、不透明混合物以及多相系统)运行的关键能力。化学反应本身会引起反应介质、邻近化合物、表面成分和/或相关化合物的键合结构发生变化,从而导致环境变化。最近开发的 FLIM 方法可以利用和解释这些变化,从而确定化合物的特征并加深对机理的理解。在此,我们考虑了 FLIM 方法目前的优势和局限性,以教程的形式讨论了影响化学体系中荧光寿命的常见因素,并战略性地分析了七个研究案例--这些案例强调了 FLIM 如何为理解化学反应机理、中间产物、产物分布、分配、试剂作用和催化剂行为提供补充信息。从 FLIM 中获得的这些数据和见解有助于合理设计和优化合成与催化方法。
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