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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Charge Transfer between Electroactive Species Immobilized on Carbon Surfaces by Aryl Diazonium Reduction. SECM Investigations
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Charge Transfer between Electroactive Species Immobilized on Carbon Surfaces by Aryl Diazonium Reduction. SECM Investigations

机译：通过芳基重氮鎓还原固定在碳表面上的电活性物种之间的电荷转移。 SECM调查

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摘要

Electron transfers in modified polyaryl multilayers containing redox active molecules (ferrocenyl moieties) have been investigated by scanning electrochemical microscopy (SECM) in feedback mode. The modified surfaces were prepared by the electro-reduction of aryl diazonium salts that provides anchoring layers for the immobilization of the electroactive groups. Two types of anchoring films were prepared, the first with aminophenyl and the second with phenylcarboxylic acid groups, allowing us to vary the oxidation level of the electroactive film. Determination of the apparent electron transfer rates between the modified surface and a series of redox mediators displaying increasing standard potentials permits the analysis of different processes involved in the charge transfer, namely, the permeation of the organic molecules (the mediator) and the conduction mechanism. In addition to the first oxidation of the immobilized molecules by the mediator at the solution-film interface, the global oxidation kinetics involves the conduction by charge transfer between grafted ferrocenes and the reverse charge transfer reaction from the film to mediator. This last step that is required to maintain the charge balance could become a kinetic limit for the highest driving force. For the most oxidizing mediator, analyses also suggest that the aromatic layer participates in the charge transfer.
机译：已通过扫描电化学显微镜（SECM）以反馈模式研究了含有氧化还原活性分子（二茂铁基部分）的改性聚芳基多层体中的电子转移。通过电还原芳基重氮盐制备改性的表面，该芳基重氮盐为固定电活性基团提供了锚固层。制备了两种类型的锚定膜，第一种具有氨基苯基，第二种具有苯基羧酸基，这使我们能够改变电活性膜的氧化水平。确定改性表面与显示出越来越高的标准电势的一系列氧化还原介体之间的表观电子转移速率，可以分析与电荷转移有关的不同过程，即有机分子（介体）的渗透和导电机理。除了固溶分子在溶液-膜界面的首次氧化，整体氧化动力学还涉及到接枝二茂铁之间电荷转移的传导以及从薄膜到介质的逆电荷转移反应。维持电荷平衡所需的最后一步可能成为最高驱动力的动力学极限。对于最具氧化性的介体，分析还表明，芳族层参与了电荷转移。

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