Ciesielski Peter N, Scott Amanda M, Faulkner Christopher J, Berron Brad J, Cliffel David E, Jennings G Kane
Interdisciplinary Materials Science Program, Department of Chemistry, Vanderbilt University, Nashville, TN 37240, USA.
ACS Nano. 2008 Dec 23;2(12):2465-72. doi: 10.1021/nn800389k.
Plants and some types of bacteria demonstrate an elegant means to capitalize on the superabundance of solar energy that reaches our planet with their energy conversion process called photosynthesis. Seeking to harness Nature's optimization of this process, we have devised a biomimetic photonic energy conversion system that makes use of the photoactive protein complex Photosystem I, immobilized on the surface of nanoporous gold leaf (NPGL) electrodes, to drive a photoinduced electric current through an electrochemical cell. The intent of this study is to further the understanding of how the useful functionality of these naturally mass-produced, biological light-harvesting complexes can be integrated with nonbiological materials. Here, we show that the protein complexes retain their photonic energy conversion functionality after attachment to the nanoporous electrode surface and, further, that the additional PSI/electrode interfacial area provided by the NPGL allows for an increase in PSI-mediated electron transfer with respect to an analogous 2D system if the pores are sufficiently enlarged by dealloying. This increase of interfacial area is pertinent for other applications involving electron transfer between phases; thus, we also report on the widely accessible and scalable method by which the NPGL electrode films used in this study are fabricated and attached to glass and Au/Si supports and demonstrate their adaptability by modification with various self-assembled monolayers. Finally, we demonstrate that the magnitude of the PSI-catalyzed photocurrents provided by the NPGL electrode films is dependent upon the intensity of the light used to irradiate the electrodes.
植物和某些种类的细菌通过一种名为光合作用的能量转换过程,展示了一种巧妙利用到达地球的太阳能过剩的方式。为了利用大自然对这一过程的优化,我们设计了一种仿生光子能量转换系统,该系统利用固定在纳米多孔金叶(NPGL)电极表面的光活性蛋白复合物光系统I,来驱动光诱导电流通过一个电化学电池。本研究的目的是进一步了解这些天然大量生产的生物光捕获复合物的有用功能如何与非生物材料整合。在这里,我们表明蛋白复合物在附着到纳米多孔电极表面后仍保留其光子能量转换功能,此外,如果通过脱合金使孔隙充分扩大,NPGL提供的额外PSI/电极界面面积相对于类似的二维系统可使PSI介导的电子转移增加。界面面积的这种增加与涉及相之间电子转移的其他应用相关;因此,我们还报告了本研究中使用的NPGL电极膜的广泛可用且可扩展的制备方法,以及将其附着到玻璃和Au/Si支撑体上的方法,并通过用各种自组装单分子层进行修饰来证明其适应性。最后,我们证明NPGL电极膜提供的PSI催化光电流的大小取决于用于照射电极的光的强度。