Water Oxidation Catalysis: Influence of Anionic Ligands upon the Redox Properties and Catalytic Performance of Mononuclear Ruthenium Complexes

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Water Oxidation Catalysis : Influence of Anionic Ligands upon the Redox Properties and Catalytic Performance of Mononuclear Ruthenium Complexes

Tong, Lianpeng (författare): KTH,Kemi

Wang, Ying (författare): KTH,Teoretisk kemi och biologi

Duan, Lele (författare): KTH,Organisk kemi

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Xu, Yunhua (författare): KTH,Organisk kemi

Cheng, Xiao (författare): KTH,Teoretisk kemi och biologi

Fischer, Andreas (författare): KTH,Kemi

Ahlquist, Mårten S. G. (författare): KTH,Teoretisk kemi och biologi

Sun, Licheng (författare): KTH,Organisk kemi

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(creator_code:org_t)

2012-02-24
2012
Engelska.
Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 51:6, s. 3388-3398

Relaterad länk:: https://urn.kb.se/re...; visa fler...; https://doi.org/10.1...; visa färre...

Tidskriftsartikel (refereegranskat)

Abstract Ämnesord

Stäng

Aiming at highly efficient molecular catalyts for water oxidation, a mononuclear ruthenium complex Ru-II(hqc)(pic)(3) (1; H(2)hqc = 8-hydroxyquinoline-2-carboxylic acid and plc = 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 Rum state complex 1 undergoes ligand exchange of 4-picoline with water, forming the authentic water oxidation catalyst in situ. Density functional theory (DFT) was ernployed to explain how anionic ligands (hqc and pdc) facilitate the 4-picoline dissociation compared with a neutral ligand (tpy). Electrochemical measurements show that complex 1 has a much lower E(Ru-III/Ru-II) than that of reference complex 2 because of the introduction of a phenolate ligand. DFT was further used to study the influence of anionic ligands upon the redox properties of mononuclear aquaruthenium species, which are postulated to be involved in the catalysis cycle of water oxidation.

Ämnesord

NATURVETENSKAP -- Kemi (hsv//swe)
NATURAL SCIENCES -- Chemical Sciences (hsv//eng)

Nyckelord

Molecular Catalysts
Excited-States
Density
Thermochemistry
Solvation
Dioxygen
Kinetics
Energy
Cells
Dimer

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Av författaren/redakt...: Tong, Lianpeng; Wang, Ying; Duan, Lele; Xu, Yunhua; Cheng, Xiao; Fischer, Andreas; visa fler...; Ahlquist, Mårten ...; Sun, Licheng; visa färre...

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Av lärosätet: Kungliga Tekniska Högskolan

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