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dc.contributor.author
Megiatto, Jackson D.
dc.contributor.author
Antoniuk Pablant, Antaeres
dc.contributor.author
Sherman, Benjamin D.
dc.contributor.author
Kodis, Gerdenis
dc.contributor.author
Gervaldo, Miguel Andres
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dc.contributor.author
Moore, Thomas A.
dc.contributor.author
Moore, Ana L.
dc.contributor.author
Gust, Devens
dc.date.available
2023-04-20T13:45:14Z
dc.date.issued
2012-03
dc.identifier.citation
Megiatto, Jackson D.; Antoniuk Pablant, Antaeres; Sherman, Benjamin D.; Kodis, Gerdenis; Gervaldo, Miguel Andres; et al.; Mimicking the electron transfer chain in photosystem II with a molecular triad thermodynamically capable of water oxidation; National Academy of Sciences; Proceedings of the National Academy of Sciences of The United States of America; 109; 39; 3-2012; 15578-15583
dc.identifier.issn
0027-8424
dc.identifier.uri
http://hdl.handle.net/11336/194735
dc.description.abstract
In the photosynthetic photosystem II, electrons are transferred from the manganese-containing oxygen evolving complex (OEC) to the oxidized primary electron-donor chlorophyll P680•+ by a proton-coupled electron transfer process involving a tyrosine-histidine pair. Proton transfer from the tyrosine phenolic group to a histidine nitrogen positions the redox potential of the tyrosine between those of P680•+ and the OEC. We report the synthesis and time-resolved spectroscopic study of a molecular triad that models this electron transfer. The triad consists of a high-potential porphyrin bearing two pentafluorophenyl groups (PF10), a tetracyanoporphyrin electron acceptor (TCNP), and a benzimidazole-phenol secondary electron-donor (Bi-PhOH). Excitation of PF10 in benzonitrile is followed by singlet energy transfer to TCNP (τ = 41 ps), whose excited state decays by photoinduced electron transfer (τ = 830 ps) to yield Bi-PhOH-PF 10•+-TCNP•-. A second electron transfer reaction follows (τ < 12 ps), giving a final state postulated as BiH+-PhO•-PF10-TCNP•-, in which the phenolic proton now resides on benzimidazole. This final state decays with a time constant of 3.8 μs. The triad thus functionally mimics the electron transfers involving the tyrosine-histidine pair in PSII. The final charge-separated state is thermodynamically capable of water oxidation, and its long lifetime suggests the possibility of coupling systems such as this system to water oxidation catalysts for use in artificial photosynthetic fuel production.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
National Academy of Sciences
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dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
BIOMIMICRY
dc.subject
PHOTOCHEMISTRY
dc.subject.classification
Química Orgánica
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dc.subject.classification
Ciencias Químicas
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dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
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dc.title
Mimicking the electron transfer chain in photosystem II with a molecular triad thermodynamically capable of water oxidation
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2023-04-20T12:33:10Z
dc.journal.volume
109
dc.journal.number
39
dc.journal.pagination
15578-15583
dc.journal.pais
Estados Unidos
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dc.description.fil
Fil: Megiatto, Jackson D.. Arizona State University; Estados Unidos
dc.description.fil
Fil: Antoniuk Pablant, Antaeres. Arizona State University; Estados Unidos
dc.description.fil
Fil: Sherman, Benjamin D.. Arizona State University; Estados Unidos
dc.description.fil
Fil: Kodis, Gerdenis. Arizona State University; Estados Unidos
dc.description.fil
Fil: Gervaldo, Miguel Andres. Universidad Nacional de Río Cuarto; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina
dc.description.fil
Fil: Moore, Thomas A.. Arizona State University; Estados Unidos
dc.description.fil
Fil: Moore, Ana L.. Arizona State University; Estados Unidos
dc.description.fil
Fil: Gust, Devens. Arizona State University; Estados Unidos
dc.journal.title
Proceedings of the National Academy of Sciences of The United States of America
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dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://www.pnas.org/doi/10.1073/pnas.1118348109
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1073/pnas.1118348109
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