Photocurrent Generation from Surface Assembled Photosystem I on Alkanethiol Modified Electrodes
Photocurrent Generation from Surface Assembled Photosystem I on Alkanethiol Modified Electrodes
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DOI：
10.1021/la304477u
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发表时间：
2013-02-19
期刊：
影响因子：
3.9
通讯作者：
Lundgren, Cynthia A.
中科院分区：
文献类型：
--
作者：
Manocchi, Amy K.;Baker, David R.;Lundgren, Cynthia A.
光系统I （PSI）是光合作用电子传递的关键组成部分，因为它的光诱导电子转移到可溶性电子受体铁氧还蛋白。这项工作证明了将表面组装的蓝藻三聚体PSI复合物整合到光驱动电流产生的生物杂交系统中。具体来说，这项工作证明了通过电泳沉积改进PSI的组装，具有可控的表面组装PSI密度，在不同的自组装烷硫醇单层上。使用人工电子供体和受体(Os（bpy)(2)Cl-2和甲基紫胶），我们演示了单个PSI层产生的光电流，该层在至少三小时的间歇照明下保持光活性。由不同烷硫醇（己硫醇、氨基己硫醇、巯基己醇和巯基己酸）组成的生物杂化体系的光电化学比较表明，在带负电的SAM表面上，PSI产生的光电流比带正电的SAM表面增强了近5倍。这些结果讨论了如何PSI定向电沉积在SAM上。
Photosystem I (PSI) is a key component of oxygenic photosynthetic electron transport because of its light-induced electron transfer to the soluble electron acceptor ferredoxin. This work demonstrates the incorporation of surface assembled cyanobacterial trimeric PSI complexes into a biohybrid system for light-driven current generation. Specifically, this work demonstrates the improved assembly of PSI via electrophoretic deposition, with controllable surface assembled PSI density, on different self-assembled alkanethiol monolayers. Using artificial electron donors and acceptors (Os(bpy)(2)Cl-2 and methyl viologen) we demonstrate photocurrent generation from a single PSI layer, which remains photoactive for at least three hours of intermittent illumination. Photoelectrochemical comparison of the biohybrid systems assembled from different alkanethiols (hexanethiol, aminohexanethiol, mercaptohexanol, and mercaptohexanoic acid) reveals that the PSI generated photocurrent is enhanced by almost 5 times on negatively charged SAM surfaces as compared to positively charged surfaces. These results are discussed in light of how PSI is oriented upon electrodeposition on a SAM.