Water oxidation catalysis: influence of anionic ligands upon the redox properties and catalytic performance of mononuclear ruthenium complexes

Inorganic Chemistry
Lianpeng TongLicheng Sun

Abstract

Aiming at highly efficient molecular catalysts for water oxidation, a mononuclear ruthenium complex Ru(II)(hqc)(pic)(3) (1; H(2)hqc = 8-hydroxyquinoline-2-carboxylic acid and pic = 4-picoline) containing negatively charged carboxylate and phenolate donor groups has been designed and synthesized. As a comparison, two reference complexes, Ru(II)(pdc)(pic)(3) (2; H(2)pdc = 2,6-pyridine-dicarboxylic acid) and Ru(II)(tpy)(pic)(3) (3; tpy = 2,2':6',2"-terpyridine), have also been prepared. All three complexes are fully characterized by NMR, mass spectrometry (MS), and X-ray crystallography. Complex 1 showed a high efficiency toward catalytic water oxidation either driven by chemical oxidant (Ce(IV) in a pH 1 solution) with a initial turnover number of 0.32 s(-1), which is several orders of magnitude higher than that of related mononuclear ruthenium catalysts reported in the literature, or driven by visible light in a three-component system with [Ru(bpy)(3)](2+) types of photosensitizers. Electrospray ionization MS results revealed that at the Ru(III) state complex 1 undergoes ligand exchange of 4-picoline with water, forming the authentic water oxidation catalyst in situ. Density functional theory (DFT) was employed to explain how an...Continue Reading

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Citations

Feb 16, 2013·Inorganic Chemistry·Lianpeng TongLicheng Sun
Jul 15, 2015·Journal of Photochemistry and Photobiology. B, Biology·Long-Xin XueKe-Zhi Wang
Aug 12, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Ying Wang, Mårten S G Ahlquist
Jan 10, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Zhongkai LuLicheng Sun
Jun 2, 2017·Chemical Science·Lianpeng Tong, Randolph P Thummel
Oct 21, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Qi LuoJing Zhang
Jul 20, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Zhongkai LuLicheng Sun
Nov 18, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Andrey ShatskiyBjörn Åkermark
Aug 8, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Yukun ZhaoMindong Chen
Jul 25, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Chuanjun WangWen-Fu Fu
Nov 1, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Anna IgnaszakCarl Redshaw
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Oct 30, 2014·Chemical Reviews·Markus D KärkäsBjörn Åkermark
Apr 22, 2016·Inorganic Chemistry·Yangyang ZhangXuesong Wang

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