TY - JOUR
T1 - Water oxidation by mononuclear ruthenium complexes with TPA-based ligands
AU - Radaram, Bhasker
AU - Ivie, Jeffrey A.
AU - Singh, Wangkheimayum Marjit
AU - Grudzien, Rafal M.
AU - Reibenspies, Joseph H.
AU - Webster, Charles Edwin
AU - Zhao, Xuan
PY - 2011/11/7
Y1 - 2011/11/7
N2 - The synthesis, characterization, and water oxidation activity of mononuclear ruthenium complexes with tris(2-pyridylmethyl)amine (TPA), tris(6-methyl-2-pyridylmethyl)amine (Me 3TPA), and a new pentadentate ligand N,N-bis(2-pyridinylmethyl)-2,2′-bipyridine-6-methanamine (DPA-Bpy) have been described. The electrochemical properties of these mononuclear Ru complexes have been investigated by both experimental and computational methods. Using Ce IV as oxidant, stoichiometric oxidation of water by [Ru(TPA)(H 2O) 2] 2+ was observed, while Ru(Me 3TPA)(H 2O) 2] 2+ has much less activity for water oxidation. Compared to [Ru(TPA)(H 2O) 2] 2+ and [Ru(Me 3TPA)(H 2O) 2] 2+, [Ru(DPA-Bpy)(H 2O)] 2+ exhibited 20 times higher activity for water oxidation. This study demonstrates a new type of ligand scaffold to support water oxidation by mononuclear Ru complexes.
AB - The synthesis, characterization, and water oxidation activity of mononuclear ruthenium complexes with tris(2-pyridylmethyl)amine (TPA), tris(6-methyl-2-pyridylmethyl)amine (Me 3TPA), and a new pentadentate ligand N,N-bis(2-pyridinylmethyl)-2,2′-bipyridine-6-methanamine (DPA-Bpy) have been described. The electrochemical properties of these mononuclear Ru complexes have been investigated by both experimental and computational methods. Using Ce IV as oxidant, stoichiometric oxidation of water by [Ru(TPA)(H 2O) 2] 2+ was observed, while Ru(Me 3TPA)(H 2O) 2] 2+ has much less activity for water oxidation. Compared to [Ru(TPA)(H 2O) 2] 2+ and [Ru(Me 3TPA)(H 2O) 2] 2+, [Ru(DPA-Bpy)(H 2O)] 2+ exhibited 20 times higher activity for water oxidation. This study demonstrates a new type of ligand scaffold to support water oxidation by mononuclear Ru complexes.
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U2 - 10.1021/ic200050g
DO - 10.1021/ic200050g
M3 - Article
C2 - 21999861
AN - SCOPUS:80155134031
SN - 0020-1669
VL - 50
SP - 10564
EP - 10571
JO - Inorganic Chemistry
JF - Inorganic Chemistry
IS - 21
ER -