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有序介孔碳功能化四硫富瓦烯的氧电催化还原。

Electrocatalytic reduction of oxygen at ordered mesoporous carbon functionalized with tetrathiafulvalene.

机构信息

Faculty of Chemistry, Northeast Normal University, Changchun, 130024, China.

出版信息

Analyst. 2010 Mar;135(3):621-9. doi: 10.1039/b919532g. Epub 2010 Jan 13.

Abstract

A novel ordered mesoporous carbon-tetrathiafulvalene composite is synthesized. It is based on host-guest chemistry which utilizes synergic interactions between a nanostructured matrix of ordered mesoporous carbon (OMC) and the excellent electron donor properties of tetrathiafulvalene (TTF). It has been found that some interesting properties of OMC are improved. Especially the density of the edge plane-like defective sites, important groups responsible for the electrocatalytic activity towards some molecules, is increased on OMC-TTF composite. Moreover, this new material can be used to facilitate the heterogeneous electron transfer process. OMC-TTF was used, for the first time, to investigate the electrocatalytic reduction of oxygen. The results show that the electrocatalytic behavior of OMC-TTF is attributed to the unique physico-chemical properties of OMC and TTF. At the OMC-TTF modified electrode, the reduction proceeds by the direct four-electron pathway whereas at the OMC electrode the process is not direct. In order to show that the ability of OMC-TTF to promote the electron transfer can allow the application of this composite in many domains, an amperometric oxygen biosensor has been constructed based on OMC-TTF. It exhibits good response to dissolved oxygen with a large linear range and a very low detection limit. The interferences of ascorbic acid and uric acid are suppressed and the applied potential is positive enough to avoid perturbations of other electrochemically reducible compounds. The results above suggest that OMC-TTF has potential applications in the detection of dissolved oxygen and interesting properties of this composite may open up a new approach to study the electrochemical behavior of other biomolecules.

摘要

一种新型有序介孔碳-四硫富瓦烯复合材料被合成。它基于主客体化学,利用有序介孔碳(OMC)的纳米结构基质和四硫富瓦烯(TTF)优异的电子给体性质之间的协同相互作用。研究发现,一些 OMC 的有趣性质得到了改善。特别是,负责对某些分子的电催化活性的边缘平面状缺陷位的密度增加,这是 OMC-TTF 复合材料中的重要基团。此外,这种新材料可以促进异相电子转移过程。首次将 OMC-TTF 用于研究氧气的电催化还原。结果表明,OMC-TTF 的电催化行为归因于 OMC 和 TTF 的独特物理化学性质。在 OMC-TTF 修饰电极上,还原通过直接四电子途径进行,而在 OMC 电极上,该过程不是直接的。为了表明 OMC-TTF 促进电子转移的能力可以使这种复合材料在许多领域得到应用,基于 OMC-TTF 构建了一种安培型氧生物传感器。它对溶解氧具有良好的响应,线性范围大,检测限低。抗坏血酸和尿酸的干扰得到抑制,并且应用的电位足够正,以避免其他电化学可还原化合物的干扰。上述结果表明,OMC-TTF 在溶解氧的检测中有潜在的应用,并且这种复合材料的有趣性质可能为研究其他生物分子的电化学行为开辟新途径。

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