Light-Harvesting and Photocurrent Generation by Gold Electrodes Modified with Mixed Self-Assembled Monolayers of Boron-Dipyrrin and Ferrocene-Porphyrin-Fullerene Triad

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• 作者：Hiroshi Imahori ; Hiroyuki Norieda ; Hiroko Yamada ; Yoshinobu Nishimura ; Iwao Yamazaki ; Yoshiteru Sakata ; and Shunichi Fukuzumi
• 刊名：Journal of the American Chemical Society
• 出版年：2001
• 出版时间：January 10, 2001
• 年：2001
• 卷：123
• 期：1
• 页码：100 - 110
• 全文大小：171K
• 年卷期：v.123,no.1(January 10, 2001)
• ISSN：1520-5126

文摘

Three different kinds of mixed self-assembled monolayers have been prepared to mimic photosyntheticenergy and electron transfer on a gold surface. Pyrene and boron-dipyrrin were chosen as a light-harvestingmodel. The mixed self-assembled monolayers of pyrene (or boron-dipyrrin) and porphyrin (energy acceptormodel) reveal photoinduced singlet-singlet energy transfer from the pyrene (or boron-dipyrrin) to the porphyrinon the gold surface. The boron-dipyrrin has also been combined with a reaction center model, ferrocene-porphyrin-fullerene triad, to construct integrated artificial photosynthetic assemblies on a gold electrode usingmixed monolayers of the respective self-assembled unit. The mixed self-assembled monolayers on the goldelectrode have established a cascade of photoinduced energy transfer and multistep electron transfer, leadingto the production of photocurrent output with the highest quantum yield (50 ± 8%, based on the adsorbedphotons) ever reported for photocurrent generation at monolayer-modified metal electrodes and across artificialmembranes using donor-acceptor linked molecules. The incident photon-to-current efficiency (IPCE) of thephotoelectrochemical cell at 510 and 430 nm was determined as 0.6% and 1.6%, respectively. Thus, the presentsystem provides the first example of an artificial photosynthetic system, which not only mimics light-harvestingand charge separation processes in photosynthesis but also acts as an efficient light-to-current converter inmolecular devices.