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Rearranging from 6-to 7-coordination initiates the catalytic activity: An EPR study on a Ru-bda water oxidation catalyst
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry. (Sun)
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
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2017 (English)In: Coordination chemistry reviews, ISSN 0010-8545, E-ISSN 1873-3840, Vol. 346, p. 206-215Article in journal (Refereed) Published
Abstract [en]

The coordination of a substrate water molecule on a metal centered catalyst for water oxidation is a crucial step involving the reorganization of the ligand sphere. This process can occur by substituting a coordinated ligand with a water molecule or via a direct coordination of water onto an open site. In 2009, we reported an efficient ruthenium-based molecular catalyst, Ru-bda, for water oxidation. Despite the impressive improvement in catalytic activity of this type of catalyst over the past years, a lack of understanding of the water coordination still remains. Herein, we report our EPR and DFT studies on Ru-bda (triethylammonium 3-pyridine sulfonate)(2) (1) at its Ru-III oxidation state, which is the initial state in the catalytic cycle for the O-O bond formation. Our investigation suggests that at this III-state, there is already a rearrangement in the ligand sphere where the coordination of a water molecule at the 7th position (open site) takes place under acidic conditions (pH = 1.0) to form a rare 7-coordinated Ru-III species.

Place, publisher, year, edition, pages
Elsevier, 2017. Vol. 346, p. 206-215
Keywords [en]
Water oxidation, EPR, Ruthenium, Coordination, DFT
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-207807DOI: 10.1016/j.ccr.2017.02.019ISI: 000402873900014Scopus ID: 2-s2.0-85014846790OAI: oai:DiVA.org:kth-207807DiVA, id: diva2:1098592
Funder
Swedish Energy AgencySwedish Research CouncilKnut and Alice Wallenberg Foundation
Note

QC 20170608

Available from: 2017-05-24 Created: 2017-05-24 Last updated: 2018-02-27Bibliographically approved

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Duan, LeleWang, LeiLi, FushengAhlquist, Mårten S. G.Sun, Licheng

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