Electronic Structure of the CaMn4O5 Cluster in the PSII System Refined to the 1.9 Å X-ray Resolution. Possible Mechanisms of ... View Full Text


Ontology type: schema:Chapter     


Chapter Info

DATE

2013

AUTHORS

Tingyun Kuang , Congming Lu , Lixin Zhang , S. Yamanaka , K. Kanda , H. Isobe , K. Nakata , Y. Umena , K. Kawakami , J. R. Shen , N. Kamiya , M. Okumura , T. Takada , H. Nakamura , K. Yamaguchi

ABSTRACT

Broken-symmetry (BS) UB3LYP calculations have been performed for the CaMn4O5 cluster (1) in the oxygen-evolving complex (OEC) of the PSII system refined to 1.9 Å resolution by Umena, Kawakami, Kamiya, Shen to elucidate its electronic structure that is crucial for consideration of possible mechanisms of photosynthetic water splitting. Our UB3LYP computations have elucidated the position of protonated oxygen of the CaMn(III)2Mn(IV)2O4(OH) cluster (1a) at the S1 stage of Kok cycle. Starting from the newly elucidated S1 structure of 1a, we have calculated the electronic structure of proton and electron released CaMn(IV)4O5 cluster (1b) that mimics the S4 stage of the cycle. The LUMOs of 1b are depicted for pictorial understanding of electrophilic oxygen sites that are responsible for nucleophilic attack of hydroxide anion (or water) for the O-O bond formation. Implications of present computational results are discussed in relation to possible mechanisms of photosynthetic water splitting. More... »

PAGES

250-254

Book

TITLE

Photosynthesis Research for Food, Fuel and the Future

ISBN

978-3-642-32033-0
978-3-642-32034-7

Identifiers

URI

http://scigraph.springernature.com/pub.10.1007/978-3-642-32034-7_52

DOI

http://dx.doi.org/10.1007/978-3-642-32034-7_52

DIMENSIONS

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