2016
DOI: 10.1021/jacs.5b12650
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A Molecular Tetrad That Generates a High-Energy Charge-Separated State by Mimicking the Photosynthetic Z-Scheme

Abstract: The oxygenic photosynthesis of green plants, green algae, and cyanobacteria is the major provider of energy-rich compounds in the biosphere. The so-called "Z-scheme" is at the heart of this "engine of life". Two photosystems (photosystem I and II) work in series to build up a higher redox ability than each photosystem alone can provide, which is necessary to drive water oxidation into oxygen and NADP(+) reduction into NADPH with visible light. Here we show a mimic of the Z-scheme with a molecular tetrad. The t… Show more

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Cited by 67 publications
(54 citation statements)
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“…Accordingly, quinones ( Q ) are able to engage in weak noncovalent interactions, whereas their reduction to the semiquinone ( SQ ) state increases this ability by several orders of magnitude, enabling them to act as strong hydrogen bond acceptors that interact with the neighboring protein residues carrying hydrogen bond donors (HBD), such as His (Figure a) . These redox‐controlled noncovalent interactions can trigger conformational changes in the reaction center that modify the redox environment and further play a role in the formation of the chemiosmotic gradient required for the operation of the ATP synthase, which ultimately converts the electromagnetic inputs into chemical energy …”
Section: Introductionmentioning
confidence: 99%
“…Accordingly, quinones ( Q ) are able to engage in weak noncovalent interactions, whereas their reduction to the semiquinone ( SQ ) state increases this ability by several orders of magnitude, enabling them to act as strong hydrogen bond acceptors that interact with the neighboring protein residues carrying hydrogen bond donors (HBD), such as His (Figure a) . These redox‐controlled noncovalent interactions can trigger conformational changes in the reaction center that modify the redox environment and further play a role in the formation of the chemiosmotic gradient required for the operation of the ATP synthase, which ultimately converts the electromagnetic inputs into chemical energy …”
Section: Introductionmentioning
confidence: 99%
“…[1] Several innovative photoelectrochemical cells for water splitting have been proposed since the pioneering work by Fujishima and Honda. [7][8][9] Molecular ruthenium complexes (as photosensitizers and/or WOCs) remain the most widely used despite their high cost and easy decomposition under photocatalytic conditions. This approach has further been expanded by integrating suitable donor and acceptor units to prepare molecular triads, tetrads,a nd pentads for efficient charge separation.…”
mentioning
confidence: 99%
“…They can be reduced to the semiquinone radical anion ( SQ ) and quinone dianion ( Q 2− ) states; protonation of the latter leads to the formation of hydroquinone ( HQ ; Figure c). These intermediates alter the environment in the photosynthetic reaction center and contribute to the photosynthetic machinery, which converts light into chemical energy (Figure a) . The process is mediated by the conformational changes in the reaction center, as a result of the interaction of the peptide backbone (i.e., His units, H; Figure b) with the ubiquinone cofactors ( Q A and Q B ; Figure b), which occurs through stronger hydrogen bonding (HB) in the SQ state .…”
Section: Redox‐controlled Resorcin[4]arenesmentioning
confidence: 99%