Chemical and Photochemical Water Oxidation Catalyzed by Mononuclear Ruthenium Complexes with a Negatively Charged Tridentate Ligand | Zendy

Duan Lele | Zendy; Xu Yunhua | Zendy; Gorlov Mikhail | Zendy; Tong Lianpeng | Zendy; Andersson Samir | Zendy; Sun Licheng | Zendy

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Chemical and Photochemical Water Oxidation Catalyzed by Mononuclear Ruthenium Complexes with a Negatively Charged Tridentate Ligand

Author(s) -

Duan Lele,

Xu Yunhua,

Gorlov Mikhail,

Tong Lianpeng,

Andersson Samir,

Sun Licheng

Publication year - 2010

Publication title -

chemistry – a european journal

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 1.687

H-Index - 242

eISSN - 1521-3765

pISSN - 0947-6539

DOI - 10.1002/chem.200902603

Subject(s) - ruthenium , catalysis , chemistry , ligand (biochemistry) , photochemistry , turnover number , picoline , redox , medicinal chemistry , inorganic chemistry , organic chemistry , receptor , pyridine , biochemistry

Two mononuclear ruthenium complexes [RuL(pic) 3 ] ( 1 ) and [RuL(bpy)(pic)] ( 2 ) (H 2 L=2,6‐pyridinedicarboxylic acid, pic=4‐picoline, bpy=2,2′‐bipyridine) have been synthesized and fully characterized. Both complexes could promote water oxidation chemically and photochemically. Compared with other known ruthenium‐based water oxidation catalysts using [Ce(NH 4 ) 2 (NO 3 ) 6 ] (Ce IV ) as the oxidant in solution at pH 1.0, complex 1 is one of the most active catalysts yet reported with an initial rate of 0.23 turnover s −1 . Under acidic conditions, the equatorial 4‐picoline in complex 1 dissociates first. In addition, ligand exchange in 1 occurs when the Ru III state is reached. Based on the above observations and MS measurements of the intermediates during water oxidation by 1 using Ce IV as oxidant, [RuL(pic) 2 (H 2 O)] + is proposed as the real water oxidation catalyst.

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