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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Electron Transfer Triggers Fast Dimer/Monomer Switching of Pyridinium and Quinoliniym Cations
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Electron Transfer Triggers Fast Dimer/Monomer Switching of Pyridinium and Quinoliniym Cations

机译：电子转移触发吡啶和喹啉正阳离子的快速二聚体/单体转换

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摘要

N-Heteroaromatic cations with quaternary pyr-idine-type nitrogen atoms have a rich application potential due to their bioactivity, fluorescence, and redox properties. Reactivity of radicals formed by reduction of such compounds is of key importance. We report the electron transfer mechanism of four novel compounds containing pyridinium, quinolinium, and benzothiazolium moiety. The reduction of pyridinium and quinolinium derivatives by one electron yields radicals that very rapidly form σ-dimers. Dimers can be converted to parent cations by oxidation, which proceeds at considerably higherpotentials. Hence the dimerization can be reversibly switched by application of the appropriate electrode potential. In contrast, in benzothiazolium derivative the electron transfer yields a stable radical in which the follow-up dimerization reaction is completely blocked. Analysis of experimental data as well as theoretical models led to the identification of dimerization sites in reduced pyridinium and quinolinium species. We show the advantage of using the combination of electrochemical impedance data and simulation of cyclic voltammograms for estimation of kinetic parameters of the heterogeneous electron transfer rates and the coupled chemical reactions.
机译：具有季吡啶-型氮原子的N-杂芳族阳离子由于其生物活性，荧光和氧化还原特性而具有丰富的应用潜力。通过还原此类化合物形成的自由基的反应性至关重要。我们报告了含有吡啶鎓，喹啉鎓和苯并噻唑鎓部分的四种新型化合物的电子转移机理。吡啶鎓和喹啉鎓衍生物被一个电子还原会产生非常迅速形成σ-二聚体的自由基。二聚体可以通过氧化转化为母体阳离子，这种氧化以相当高的电势进行。因此，可以通过施加适当的电极电势来可逆地切换二聚作用。相反，在苯并噻唑鎓衍生物中，电子转移产生稳定的自由基，其中后续的二聚反应被完全阻断。通过对实验数据和理论模型的分析，可以确定还原的吡啶鎓和喹啉鎓物种中的二聚位点。我们展示了结合使用电化学阻抗数据和循环伏安图模拟来估算异质电子传输速率和耦合化学反应动力学参数的优势。

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