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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >A Comparison of Electron-Transfer Dynamics in Ionic Liquids and Neutral Solvents
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A Comparison of Electron-Transfer Dynamics in Ionic Liquids and Neutral Solvents

机译：离子液体和中性溶剂中电子转移动力学的比较

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摘要

The effect of ionic liquids on photoinduced electron-transfer reactions in a donor—bridge—acceptor system is examined for two ionic liquid solvents, 1-butyl-1-methyl-pyrrolidinium bis (trifluoromethylsulfonyl) amide and tributyl-methylammonium bis(trifluoromethylsulfonyl)amide. The results are compared with those for the same system in methanol and acetonitrile solution. Electron-transfer rates were measured using time-resolved fluorescence quenching for the donor-bridge—acceptor system comprising a 1-N,1-N-dimethylben-zene-1,4-diamine donor, a proline bridge, and a coumarin 343 acceptor. The photoinduced electron-transfer processes are in the inverted regime (—ΔG > λ) in all four solvents, with driving forces of —1.6 to —1.9 eV and estimated reorganization energies of about 1.0 eV. The observed electron-transfer kinetics have broadly distributed rates that are generally slower in the ionic liquids compared to the neutral solvents, which also have narrower rate distributions. To describe the broad distributions of electron-transfer kinetics, we use two different models: a distribution of exponential lifetimes and a discrete sum of exponential lifetimes. Analysis of the donor—acceptor electronic coupling shows that for ionic liquids this intramolecular electron-transfer reaction should be treated using a solvent-controlled electron-transfer model.
机译：针对两种离子液体溶剂，即1-丁基-1-甲基吡咯烷鎓双（三氟甲基磺酰基）酰胺和三丁基甲基铵双（三氟甲基磺酰基）酰胺，研究了离子液体对供体-桥-受体系统中光诱导的电子转移反应的影响。 。将结果与在甲醇和乙腈溶液中相同系统的结果进行比较。使用时间分辨的荧光猝灭法对供体桥-受体系统（包括1-N，1-N-二甲基苯-zene-1,4-二胺供体，脯氨酸桥和香豆素343受体）进行电子传输速率测量。在所有四种溶剂中，光诱导的电子转移过程处于倒置状态（-ΔG>λ），驱动力为-1.6至-1.9 eV，估计的重组能为约1.0 eV。观察到的电子转移动力学具有广泛分布的速率，与中性溶剂相比，在离子液体中通常较慢，中性溶剂的速率分布也较窄。为了描述电子传输动力学的广泛分布，我们使用两个不同的模型：指数寿命的分布和指数寿命的离散总和。对供体-受体电子耦合的分析表明，对于离子液体，此分子内电子转移反应应使用溶剂控制的电子转移模型进行处理。

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