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Electron-Transfer Rates in Host–Guest Assemblies at β-Cyclodextrin Monolayers
Langmuir ( IF 3.7 ) Pub Date : 2017-01-09 00:00:00 , DOI: 10.1021/acs.langmuir.6b03860 Alejandro Méndez-Ardoy 1 , Tom Steentjes 1 , Bernard A. Boukamp 1 , Pascal Jonkheijm 1 , Tibor Kudernac 1 , Jurriaan Huskens 1
Langmuir ( IF 3.7 ) Pub Date : 2017-01-09 00:00:00 , DOI: 10.1021/acs.langmuir.6b03860 Alejandro Méndez-Ardoy 1 , Tom Steentjes 1 , Bernard A. Boukamp 1 , Pascal Jonkheijm 1 , Tibor Kudernac 1 , Jurriaan Huskens 1
Affiliation
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The effect of the distance between a β-cyclodextrin (βCD) host core and a conductive substrate on the electron-transfer rate of complexed guests as well as of free-diffusing electrochemically active probes has been studied. First we have evaluated a set of short-tethered βCD adsorbates bearing different anchoring groups in order to get a reliable platform for the study of short-distance electron transfer. An electrochemically active trivalent guest was immobilized on these host monolayers in a selective and reversible manner, providing information about the packing density. Iodine- and nitrile-functionalized βCD monolayers gave coverages close to maximum packing. Electron transfer in the presence of Fe(CN)63–/4– studied by impedance spectroscopy revealed that the electron transfer of the diffusing probe was 3 orders of magnitude faster than when the βCD cores were separated from the surface by undecyl chains. When an electrochemically active guest was immobilized on the surface, electron-transfer rate measurements by cyclic voltammetry and capacitance spectroscopy showed differences of up to a factor of 8 for different βCD monolayers. These results suggest that increasing the distance between the βCD core and the underlying conductive substrate leads to a diminishing of the electron-transfer rate.
中文翻译：
β-环糊精单层宿主-客体集合中的电子传输速率
研究了β-环糊精（βCD）主体核与导电底物之间的距离对复合客体以及自由扩散电化学活性探针的电子传输速率的影响。首先，我们评估了一组带有不同锚固基团的短链βCD吸附物，以便为研究短距离电子转移提供可靠的平台。将电化学活性的三价客体以选择性和可逆的方式固定在这些主体单层上，从而提供有关堆积密度的信息。碘和腈官能化的βCD单层膜的覆盖率接近最大填充量。Fe（CN）6 3– / 4–存在下的电子转移阻抗谱研究表明，扩散探针的电子传递比通过十一烷基链将βCD核与表面分开的速度快3个数量级。当电化学活性的客体固定在表面上时，通过循环伏安法和电容光谱法进行的电子传输速率测量显示，对于不同的βCD单分子层，其差异高达8倍。这些结果表明，增加βCD核与下面的导电基底之间的距离导致电子传输速率的减小。
更新日期：2017-06-28
中文翻译：
β-环糊精单层宿主-客体集合中的电子传输速率
研究了β-环糊精（βCD）主体核与导电底物之间的距离对复合客体以及自由扩散电化学活性探针的电子传输速率的影响。首先，我们评估了一组带有不同锚固基团的短链βCD吸附物，以便为研究短距离电子转移提供可靠的平台。将电化学活性的三价客体以选择性和可逆的方式固定在这些主体单层上，从而提供有关堆积密度的信息。碘和腈官能化的βCD单层膜的覆盖率接近最大填充量。Fe（CN）6 3– / 4–存在下的电子转移阻抗谱研究表明，扩散探针的电子传递比通过十一烷基链将βCD核与表面分开的速度快3个数量级。当电化学活性的客体固定在表面上时，通过循环伏安法和电容光谱法进行的电子传输速率测量显示，对于不同的βCD单分子层，其差异高达8倍。这些结果表明，增加βCD核与下面的导电基底之间的距离导致电子传输速率的减小。
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