Theory of coupled electron and proton transfer reactions.
Theory of coupled electron and proton transfer reactions.
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DOI：
10.1021/cr1001436
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发表时间：
2010-12-08
期刊：
影响因子：
62.1
通讯作者：
Stuchebrukhov, Alexei A.
中科院分区：
文献类型：
--
作者：
Hammes-Schiffer, Sharon;Stuchebrukhov, Alexei A.
电子和质子耦合转移反应在生物能量传递机制中起着关键作用。1-3这种反应也是人工能源相关系统的基础，如燃料电池、化学传感器和其他电化学设备。生物学方面的例子包括细胞色素c氧化酶、4、5 bc1复合体、6、7和光合作用反应中心。8，9在这类体系中，电子在酶的氧化还原辅助因子之间隧穿，而耦合的质子要么通过单个氢键转移，要么沿着特殊的质子传导通道在可质子化的基团之间转移。蛋白质中的纯电子转移反应在过去已经得到了深入的研究，无论是实验上的10-17，还是理论上的。偶合反应是相对较新的反应，目前正受到该领域的关注。6、8、26-43可以区分两种类型的偶联反应。在协同的电子和质子转移反应中，ET和PT的跃迁是一步完成的。这些协同反应在文献29、30、43-45中被称为质子耦合电子转移(PCET)，但在本综述中使用的术语PCET更广泛。这种协同过程发生在质子转移通常受到限制的反应中
Coupled electron and proton transfer reactions play a key role in the mechanisms of biological energy transduction. 1-3 Such reactions are also fundamental for artificial energyrelated systems such as fuel cells, chemical sensors, and other electrochemical devices. Biological examples include, among others, cytochrome c oxidase, 4, 5 bc1 complex, 6, 7 and photosynthetic reaction centers. 8, 9 In such systems, electrons tunnel between redox cofactors of an enzyme, while the coupled protons are transferred either across a single hydrogen bond or between protonatable groups along special protonconducting channels.In this review general theories and models of coupled electron transfer and proton transfer (ET and PT) reactions are discussed. Pure electron transfer reactions in proteins have been thoroughly studied in the past, both experimentally10-17 and theoretically. 18-25 The coupled reactions are relatively new and currently are gaining attention in the field. 6, 8, 26-43 Two types of coupled reactions can be distinguished. In concerted electron and proton transfer reactions, both the ET and PT transitions occur in one step. These concerted reactions have been denoted proton-coupled electron transfer (PCET) in the literature, 29, 30, 43-45 but the term PCET is used more generally in this review. Such concerted processes occur in reactions in which proton transfer is typically limited
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