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Supramolecular electron transfer by anion binding

Title
Supramolecular electron transfer by anion binding
Authors
Fukuzumi S.Ohkubo K.D'Souza F.Sessler J.L.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2012
Journal Title
Chemical Communications
ISSN
1359-7345JCR Link
Citation
vol. 48, no. 79, pp. 9801 - 9815
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
Anion binding has emerged as an attractive strategy to construct supramolecular electron donor-acceptor complexes. In recent years, the level of sophistication in the design of these systems has advanced to the point where it is possible to create ensembles that mimic key aspects of the photoinduced electron-transfer events operative in the photosynthetic reaction centre. Although anion binding is a reversible process, kinetic studies on anion binding and dissociation processes, as well as photoinduced electron-transfer and back electron-transfer reactions in supramolecular electron donor-acceptor complexes formed by anion binding, have revealed that photoinduced electron transfer and back electron transfer occur at time scales much faster than those associated with anion binding and dissociation. This difference in rates ensures that the linkage between electron donor and acceptor moieties is maintained over the course of most forward and back electron-transfer processes. A particular example of this principle is illustrated by electron-transfer ensembles based on tetrathiafulvalene calix[4]pyrroles (TTF-C4Ps). In these ensembles, the TTF-C4Ps act as donors, transferring electrons to various electron acceptors after anion binding. Competition with non-redox active substrates is also observed. Anion binding to the pyrrole amine groups of an oxoporphyrinogen unit within various supramolecular complexes formed with fullerenes also results in acceleration of the photoinduced electron-transfer process but deceleration of the back electron transfer; again, this is ascribed to favourable structural and electronic changes. Anion binding also plays a role in stabilizing supramolecular complexes between sulphonated tetraphenylporphyrin anions ([MTPPS]4-: M = H2 and Zn) and a lithium ion encapsulated C60 (Li+@C60); the resulting ensemble produces long-lived charge-separated states upon photoexcitation of the porphyrins. © The Royal Society of Chemistry 2012.
DOI
10.1039/c2cc32848h
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자연과학대학 > 화학·나노과학전공 > Journal papers
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