Further observations on water oxidation catalyzed by mononuclear Ru(II) complexes

Inorganic Chemistry
Nattawut KaveevivitchaiRandolph P Thummel

Abstract

A family of 28 mononuclear Ru(II) complexes have been prepared and characterized by (1)H NMR, electronic absorption, and cyclic voltammetry. These complexes are studied as catalysts for water oxidation. All the catalysts possess one tridentate ligand, closely related to 2,2';6,2''-terpyridine (tpy) and may be divided into two basic types. In the type-1 catalyst, the three remaining coordination sites are occupied by a bidentate closely related to 2,2'-bipyridine (bpy) and a monodentate halogen (Br, Cl, or I) or water molecule. In the type-2 catalyst, the three remaining coordination sites are occupied by two axial 4-picoline molecules and an equatorial halogen or water. In general the type-2 catalysts are more reactive than the type-1. The type-2 iodo-catalyst shows first-order behavior and, unlike the bromo- and chloro-catalysts, does not require water-halogen exchange to show good activity. The importance of steric strain and hindrance around the metal center is examined. The introduction of three t-butyl groups at the 4, 4', and 4'' positions of tpy sometimes improves catalyst activity, but the effect does not appear to be additive.

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Citations

Feb 16, 2013·Inorganic Chemistry·Lianpeng TongLicheng Sun
Aug 31, 2013·Inorganic Chemistry·Nattawut KaveevivitchaiRandolph P Thummel
Dec 25, 2013·Inorganic Chemistry·Lars KohlerRandolph P Thummel
Jul 15, 2015·Journal of Photochemistry and Photobiology. B, Biology·Long-Xin XueKe-Zhi Wang
Mar 26, 2016·Inorganic Chemistry·Siwas PhungsriphengAkiko Inagaki
Nov 2, 2016·Journal of the American Chemical Society·Dooshaye MoonshiramYulia Pushkar
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Jun 2, 2017·Chemical Science·Lianpeng Tong, Randolph P Thummel
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