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Water Oxidation Initiated by In Situ Dimerization of the Molecular Ru(pdc) Catalyst
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).
KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD.ORCID iD: 0000-0003-1662-5817
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).
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2018 (English)In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 8, no 5, p. 4375-4382Article in journal (Refereed) Published
Abstract [en]

The mononuclear ruthenium complex [Ru(pdc)L-3] (H(2)pdc = 2,6-pyridinedicarboxylic acid, L = N-heterocycles such as 4-picoline) has previously shown promising catalytic efficiency toward water oxidation, both in homogeneous solutions and anchored on electrode surfaces. However, the detailed water oxidation mechanism catalyzed by this type of complex has remained unclear. In order to deepen understanding of this type of catalyst, in the present study, [Ru(pdc)(py)(3)] (py = pyridine) has been synthesized, and the detailed catalytic mechanism has been studied by electrochemistry, UV-vis, NMR, MS, and X-ray crystallography. Interestingly, it was found that once having reached the Ru-IV state, this complex promptly formed a stable ruthenium dimer [Ru-III(pdc)(py)(2)-O-Ru-IV(pdc)(py)(2)](+). Further investigations suggested that the present dimer, after one pyridine ligand exchange with water to form [Ru-III(pdc)(py)(2)-O-Ru-IV(pdc)(py)(H2O)](+), was the true active species to catalyze water oxidation in homogeneous solutions.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2018. Vol. 8, no 5, p. 4375-4382
Keywords [en]
solar fuels, water oxidation, electrochemistry, ruthenium dimer, mechanism of O-O bond formation
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-231630DOI: 10.1021/acscatal.7b03768ISI: 000431727300070Scopus ID: 2-s2.0-85046695744OAI: oai:DiVA.org:kth-231630DiVA, id: diva2:1229968
Note

QC 20180702

Available from: 2018-07-02 Created: 2018-07-02 Last updated: 2018-07-02Bibliographically approved

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Duan, LeleChen, HongZhang, BiaobiaoZhang, PeiliWang, LeiLi, FushengAhlquist, Mårten S. G.Sun, Licheng

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Daniel, QuentinDuan, LeleTimmer, Brian J. J.Chen, HongWang, YingZhang, BiaobiaoZhang, PeiliWang, LeiLi, FushengAhlquist, Mårten S. G.Sun, Licheng
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School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH)Centre of Molecular Devices, CMDChemistryTheoretical Chemistry and Biology
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