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The immobilization of dinuclear copper(II) acetate complexes (Cu2(CH3COO)4 3 2H2O) on self-assembled monolayers (SAMs) of different aliphatic and aromatic thiols with oxygen and nitrogen donors at the end group is investigated on preferentially oriented (111) gold surfaces (Au(111)). The Cu species are immobilized at the outer plane of these terminal groups by the interaction of the terminal moiety of the functionalized SAMs. The highest electrochemical activity for the Cu(II)/Cu(I) redox couple is found for the metallic complexes immobilized on SAMs of short thiols, irrespective of their aliphatic or aromatic character, or the nature of the terminal group of the linking molecule, suggesting that direct tunneling is the main path for charge transfer to the Au substrate. Even though a progressive demetalation of the copper acetate complex immobilized on N-terminated SAMs by the release of Cu ions to the solution is induced by repeated potential scans, this process is negligible for Cu species immobilized on O-terminated thiols. The Cu(I)/Cu(0) reaction is not observable in the overall potential range where thiol SAMs are stable on the Au(111) surface. In contrast, this reaction is clearly visible by using nanostructured Au, a substrate that exhibits a wider potential window of SAM stability and larger capture areas than ordered smooth metal surfaces. Finally, spatial 2D and 3D confinement of the copper complex can be performed by SAMs of mixed thiols with different immobilization abilities and by building complex electrochemically active supramolecular structures. Our results are important to understand the behavior of Cu centers of enzymes, the electrochemical metallization of thin organic films with Cu, and the preparation of complex three-dimensional supramolecular Cu-containing structures with spatial order. |
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zhaoqinglu05
金虫 (小有名气)
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【答案】应助回帖
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爱与雨下(金币+2): 2012-01-28 10:43:12
爱与雨下(金币+2): 2012-01-28 10:43:12
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供参考： 固定的双核铜（II）醋酸配合物在不同的脂肪族和芳香族硫醇与氧和氮的捐助者在年底组的自组装膜（SAMS）（铜（CH3COO）3· 2H2O）是调查优先导向（111）金表面（金（111））。 铜物种是固定的终端基团的功能化自组装的相互作用，在这些终端组外平面。最高的电化学活性的铜（II）/铜（一）氧化还原夫妇发现短硫醇自组装固定的金属配合物，不论其脂肪族或芳香族的性格，或连接分子的终端组的性质，表明直接隧道是电荷转移到金基板的主要路径。醋酸铜复杂的渐进demetalation即使对N -终止自组装固定到解决方案中的铜离子的释放是通过反复的潜在扫描诱导，这个过程是可以忽略不计固定在O型终止硫醇的铜物种。在Cu（I）/铜（0）的反应是观察不到的巯基自组装在Au（111）表面的稳定的整体潜力范围。相反，这种反应是使用纳米金清晰可见，具有更广泛的SAM的稳定性和更大的捕获地区比下令光滑的金属表面的电位窗基板。最后，空间的二维和三维铜配合物的约束，可以执行不同的固定能力的混合硫醇自组装，并通过建立复杂的电化学活性的超分子结构。我们的结果是重要的，了解酶，薄的有机薄膜与铜的电化学金属，并编制了复杂的三维超分子结构与空间秩序含有铜铜中心的行为 |
2楼2012-01-26 11:40:36
zhaoqinglu05
金虫 (小有名气)
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3楼2012-01-26 11:43:11
