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Why nature chose the Mn4CaO5 cluster as water-splitting catalyst in photosystem II: a new hypothesis for the mechanism of O-O bond formation
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.ORCID iD: 0000-0002-4093-1251
KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.ORCID iD: 0000-0002-4521-2870
2018 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 47, no 41, p. 14381-14387Article, review/survey (Refereed) Published
Abstract [en]

Resolving the questions, namely, the selection of Mn by nature to build the oxygen-evolving complex (OEC) and the presence of a cubic Mn3CaO4 structure in OEC coupled with an additional dangling Mn (Mn4) via mu-O atom are not only important to uncover the secret of water oxidation in nature, but also essential to achieve a blueprint for developing advanced water-oxidation catalysts for artificial photosynthesis. Based on the important experimental results reported so far in the literature and on our own findings, we propose a new hypothesis for the water oxidation mechanism in OEC. In this new hypothesis, we propose for the first time, a complete catalytic cycle involving a charge-rearrangement-induced Mn-VII-dioxo species on the dangling Mn4 during the S-3 -> S-4 transition. Moreover, the O-O bond is formed within this Mn-VII-dioxo site, which is totally different from that discussed in other existing proposals.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2018. Vol. 47, no 41, p. 14381-14387
National Category
Inorganic Chemistry
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URN: urn:nbn:se:kth:diva-241340DOI: 10.1039/c8dt01931bISI: 000454842000001PubMedID: 30129959Scopus ID: 2-s2.0-85055182383OAI: oai:DiVA.org:kth-241340DiVA, id: diva2:1280804
Note

QC 20190121

Available from: 2019-01-21 Created: 2019-01-21 Last updated: 2019-01-21Bibliographically approved

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Zhang, BiaobiaoSun, Licheng

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