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Volume 155, 2012
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Accumulative electron transfer: Multiple charge separation in artificial photosynthesis

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Abstract

To achieve artificial photosynthesis it is necessary to couple the single-electron event of photoinduced charge separation with the multi-electron reactions of fuel formation and water splitting. Therefore, several rounds of light-induced charge separation are required to accumulate enough redox equivalents at the catalytic sites for the target chemistry to occur, without any sacrificial donors or acceptors other than the catalytic substrates. Herein, we discuss the challenges of such accumulative electron transfer in molecular systems. We present a series of closely related systems base on a RuII-polypyridine photosensitizer with appended triaryl-amine or oligo-triaryl-amine donors, linked to nanoporous TiO2 as the acceptor. One of the systems, based on dye 4, shows efficient accumulative electron transfer in high overall yield resulting in the formation of a two-electron charge-separated state upon successive excitation by two photons. In contrast, the other systems do not show accumulative electron transfer because of different competing reactions. This illustrates the difficulties in designing successful systems for this still largely unexplored type of reaction scheme.

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Article information


Submitted
04 May 2011
Accepted
17 May 2011
First published
18 Oct 2011

Faraday Discuss., 2012,155, 233-252
Article type
Paper

Accumulative electron transfer: Multiple charge separation in artificial photosynthesis

S. Karlsson, J. Boixel, Y. Pellegrin, E. Blart, H. Becker, F. Odobel and L. Hammarström, Faraday Discuss., 2012, 155, 233
DOI: 10.1039/C1FD00089F

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