Proton-Coupled Electron Transfer

被引:1394
作者
Weinberg, David R. [2 ,3 ]
Gagliardi, Christopher J. [2 ]
Hull, Jonathan F. [2 ]
Murphy, Christine Fecenko [1 ]
Kent, Caleb A. [2 ]
Westlake, Brittany C. [4 ]
Paul, Amit [2 ]
Ess, Daniel H. [2 ]
McCafferty, Dewey Granville [1 ]
Meyer, Thomas J. [2 ]
机构
[1] Duke Univ, Dept Chem, Levine Sci Res Ctr B219, Durham, NC 27708 USA
[2] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA
[3] Colorado Mesa Univ, Dept Phys & Environm Sci, Grand Junction, CO 81501 USA
[4] Amer Chem Soc, Washington, DC 20036 USA
基金
美国国家科学基金会; 美国国家卫生研究院;
关键词
CYTOCHROME-C-OXIDASE; GREEN FLUORESCENT PROTEIN; OXYGEN-EVOLVING COMPLEX; HYDROGEN-ATOM TRANSFER; EXCITED-STATE DYNAMICS; REDOX-ACTIVE TYROSINE; GLASSY-CARBON ELECTRODE; ASYMMETRIC TRANSFER HYDROGENATION; ELECTROCHEMICAL CONCERTED PROTON; PHOTOSYNTHETIC WATER OXIDATION;
D O I
10.1021/cr200177j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Proton-coupled electron transfer (PCET) has a major role in chemistry and biology and its implications for catalysis and energy conversion. Photosynthesis is a spectacular example of PCET in action with the transfer of 24 e- and 24 H+ driven by at least 48 photons. In PCET half reactions, variations in pH influence driving force. Both HAT (H-atom transfer) and EPT (electron-proton transfer) are elementary steps by which PCET reactions can occur. In H-atom transfer (HAT), both the transferring electron and proton come from the same bond in one of the reactants. Multiple Site Electron-Proton Transfer (MS-EPT) is microscopically more complex than electron or proton transfer. It shares with electron transfer requirements for medium and intramolecular reorganization but with the additional complexity of a coupled proton transfer. PCET plays a critical role in many enzymatic pathways that control life such as photosynthesis, respiration, and DNA repair.
引用
收藏
页码:4016 / 4093
页数:78
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