Water Oxidation Initiated by In Situ Dimerization of the Molecular Ru(pdc) Catalyst

Timmer, Brian J. J. (author): KTH,Skolan för kemi, bioteknologi och hälsa (CBH)

Luo, Xiaodan (author): Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China.

Sun, Junliang (author): Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China.

(creator_code:org_t)

2018-03-28
2018
English.
In: ACS Catalysis. - : AMER CHEMICAL SOC. - 2155-5435. ; 8:5, s. 4375-4382

Related links:: https://urn.kb.se/re...; show more...; https://doi.org/10.1...; show less...

Abstract Subject headings

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.

By the author/editor: Daniel, Quentin; Duan, Lele; Timmer, Brian J. ...; Chen, Hong; Luo, Xiaodan; Ambre, Ram; show more...; Wang, Ying; Zhang, Biaobiao; Zhang, Peili; Wang, Lei; Li, Fusheng, 198 ...; Sun, Junliang; Ahlquist, Mårten ...; Sun, Licheng, 19 ...; show less...

About the subject

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Organic Chemistr ...

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