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首页> 外文期刊>Annual Review of Analytical Chemistry >Concerted Proton-Electron Transfers: Fundamentals and Recent Developments
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Concerted Proton-Electron Transfers: Fundamentals and Recent Developments

机译：协调的质子-电子转移：基本原理和最新发展

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Proton-coupled electron transfers (PCET) are ubiquitous in natural and synthetic processes. This review focuses on reactions where the two events are concerted. Semiclassical models of such reactions allow their kinetic characterization through activation versus driving force relationships, estimates of reorganization energies, effects of the nature of the proton acceptor, and H/D kinetic isotope effect as well as their discrimination from stepwise pathways. Several homogeneous reactions (through stopped-flow and laser flash-quench techniques) and electrochemical processes are discussed in this framework. Once the way has been rid of the improper notion of pH-dependent driving force, water appears as a remarkable proton acceptor in terms of reorganization energy and pre-exponential factor, thanks to its H-bonded and H-bonding properties, similarly to purposely synthesized "H-bond train" molecules. The most recent developments are in modeling and description of emblematic concerted proton-electron transfer (CPET) reactions associated with the breaking of a heavy-atom bond in an all-concerted process.
机译：质子耦合电子转移（PCET）在自然和合成过程中无处不在。这篇综述着重于两个事件协调一致的反应。这种反应的半经典模型允许通过激活与驱动力之间的关系来表征其动力学特性，估计重组能量，质子受体性质的影响以及H / D动力学同位素效应以及它们与逐步途径的区别。在此框架中讨论了几种均相反应（通过停止流和激光骤冷技术）和电化学过程。一旦摆脱了不正确的pH依赖驱动力概念，就其重组能和预指数因子而言，由于其H键和H键性质，水似乎是一个显着的质子受体，这与有目的的相似。合成的“ H键链”分子。最近的发展是在建模和描述具有代表性的协调一致的质子电子转移（CPET）反应中，该反应与在所有过程中破坏重原子键有关。

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