Controllable Electrochemical Activities by Oxidative Treatment toward Inner Sphere Redox Systems at N-doped Hydrogenated Amorphous Carbon Films
Controllable Electrochemical Activities by Oxidative Treatment toward Inner Sphere Redox Systems at N-doped Hydrogenated Amorphous Carbon Films
复制标题
N掺杂氢化非晶碳薄膜内球氧化还原系统氧化处理的可控电化学活性
DOI：
10.1155/2012/369130
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发表时间：
2012
影响因子：
1.8
通讯作者：
Kensuke Honda
中科院分区：
文献类型：
--
作者：
Yoriko Tanaka;Hiroshi Naragino;Kosuke Yoshinaga;Akira Nakahara;Takeshi Kondo;Akira Fujishima;Kensuke Honda
氮掺杂氢化非晶碳薄膜（a-CNH，N掺杂DLC）表面对内球氧化还原物质的电化学活性可以通过改变表面终止来控制。在氧等离子体处理的 N 掺杂 DLC 表面 (O-DLC) 上，生成了含有碳与氧双键 (C=O) 的表面官能团，从而改善了极性分子的吸附。通过氧化处理，多巴胺（DA）带正电的内球氧化还原分析物在 N 掺杂 DLC 表面的电子转移速率可以得到提高。对于 2,4-二氯苯酚的氧化还原反应，通过形成钝化膜而不可避免地导致阳极表面结垢，DLC 表面表现出明显更高的电极性能稳定性和再现性。这是由于通过施加较高电势，钝化膜发生电化学分解，而没有析氧的干扰。 N 掺杂 DLC 薄膜可以作为可极化电极表面，具有更高的反应活性和对内球氧化还原物质的更高稳定性。利用O-DLC表面这些可控的电化学反应性，可以实现DA和尿酸混合溶液中DA的选择性检测。
The electrochemical activity of the surface of Nitrogen‐doped hydrogenated amorphous carbon thin films (a‐CNH, N‐doped DLC) toward the inner sphere redox species is controllable by modifying the surface termination. At the oxygen plasma treated N‐doped DLC surface (O‐DLC), the surface functional groups containing carbon doubly bonded to oxygen (C=O), which improves adsorption of polar molecules, were generated. By oxidative treatment, the electron‐transfer rate for dopamine (DA) positively charged inner‐sphere redox analyte could be improved at the N‐doped DLC surface. For redox reaction of 2,4‐dichlorophenol, which induces an inevitable fouling of the anode surface by forming passivating films, the DLC surfaces exhibited remarkably higher stability and reproducibility of the electrode performance. This is due to the electrochemical decomposition of the passive films without the interference of oxygen evolution by applying higher potential. The N‐doped DLC film can offer benefits as the polarizable electrode surface with the higher reactivity and higher stability toward inner‐sphere redox species. By making use of these controllable electrochemical reactivity at the O‐DLC surface, the selective detection of DA in the mixed solution of DA and uric acid could be achieved.