In 2009, Sun's group introduced a novel mononuclear ruthenium water oxidation catalyst containing a tetradentate 2,2'-bipyridine-6,6'-dicarboxylate ligand and two axial 4-picoline ligands.1 This catalyst shows substantial water oxidation activity in the presence of ceric ammonium nitrate (CAN) as a sacrificial oxidant and using cyclic voltammetry performed in neutral pH. A number of literature examples show that the electronic nature of ligands bound to a metal can have a significant influence on the stability of metal oxidation states.2-6 With the implication of higher metal oxidation states in catalytic water oxidation, our group has become interested in exploring the effect of varying the electronic nature of 6,6' substituents on 2,2'-bipyridyl Sun-type ruthenium complexes. This presentation will discuss the synthesis, acid-base properties, electrochemistry, and catalytic water oxidation activity of ruthenium complexes supported by a number of 2,2'-bipyridyl tetradentate ligands with different 6,6' substituents.References:[1] L. Duan, A. Fischer, Y. Xu, and L. Sun, J. Am. Chem. Soc. 131 (2009) 10397[2] Z. Deng, H. Tseng, R. Zong, D. Wang, and R.P. Thummel, Inorg. Chem. 47 (2008) 1835[3] P. Comba, M. Morgen, and H. Wadepohl, Inorg. Chem.  52 (2013) 6481[4] L. Duan, Y. Xu, M. Gorlov, L. Tong, S. Andersson, and L. Sun, Chem. Eur. J. 16 (2010) 4659[5] L. Tong, Y. Wang, L. Duan, Y. Xu, X. Cheng, A. Fischer, M.S.G. Ahlquist, L. Sun, Inorg. Chem. 51 (2012) 3388[6] L. Wang, L. Duan, B. Stewart, M. Pu, J. Liu, T. Privalov, and L. Sun, J. Am. Chem. Soc. 134 (2012) 18868

Exploring the effect of varying the 6,6' substituents on 2,2'-bipyridyl ruthenium complexes for water oxidation

248th National Meeting (2014)

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