NDLI: Exhaustive oxidation of a nickel dithiolate complex: some mechanistic insights en route to sulfate formation

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Exhaustive oxidation of a nickel dithiolate complex: some mechanistic insights en route to sulfate formation

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Hosler, Erik R. Maroney, Michael J. Herbst, Robert W. Chohan, Balwant S.
Description	Author Affiliation: Hosler ER ( Department of Chemistry & Biochemistry, Susquehanna University, Selinsgrove, Pennsylvania 17870, USA.)
Abstract	A study of the step-wise oxidation of a Ni(II) diaminodithiolate complex through the formation of sulfate, the ultimate sulfur oxygenate, is reported. Controlled oxygenations or peroxidations of a neutral, planar, tetracoordinate, low-spin Ni(II) complex of a $N_{2}S_{2}-donor$ ligand , (N,N′-dimethyl-N-N′-bis(2-mecaptoethyl)-1,3-propanediaminato) nickel(II) (1), led to a series of sulfur oxygenates that have been isolated and characterized by ESI-MS and single-crystal X-ray diffraction . A monosulfenate complex (2) was detected by ESI-MS as a product of oxidation with one equivalent of $H_{2}O_{2}.$ However, this complex proved too unstable to isolate. Reaction of the dithiolate (1) with two equivalents of $H_{2}O_{2}$ or one $O_{2}$ molecule leads to the formation of a monosulfinate complex (3), which was isolated and fully characterized by crystallography . The oxidation product of the monosulfinate (3) produced with either $O_{2}$ or $H_{2}O_{2}$ is an interesting dimeric complex containing both sulfonate and thiolate ligands (4), this complex was fully characterized by crystallography , details of which were reported earlier by us. A disulfonate complex (7) is produced by reaction of 1 in the presence of $O_{2}$ or by reaction with exactly six equivalents of $H_{2}O_{2}.$ This complex was isolated and also fully characterized by crystallography . Possible intermediates in the conversion of the monosulfinate complex (3) to the disulfonate complex (7) include complexes with mixed sulfonate/sulfenate (5) or sulfonate/sulfinate (6) ligands . Complex 5, a four-oxygen adduct of 1, was not detected, but the sulfonate/sulfinate complex (6) was isolated and characterized. The oxidation chemistry of 1 is very different from that reported for other planar $cis-N_{2}S_{2}$ Ni(II) complexes including N,N′-dimethyl-N-N′-bis(2-mecaptoethyl)-1,3-ethylenediaminato) nickel(II), (8), and N,N'-bis(mercaptoethyl)-1,5-diazacyclooctane nickel(II). To address the structural aspects of the reactivity differences, the crystal structure of 8 was also determined. A comparison of the structures of planar Ni(II) complexes containing cis-dithiolate ligands , strongly suggests that the differences in reactivity are determined in part by the degree of flexibility that is allowed by the NN' chelate ring.
ISSN	14779226
Issue Number	3
Volume Number	41
e-ISSN	13645447
Journal	Dalton Trans.
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2012-01-21
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Nickel Chemistry Sulfates Sulfhydryl Compounds Hydrogen Peroxide Molecular Structure Oxidation-Reduction Oxygen Spectrometry, Mass, Electrospray Ionization Methods X-Ray Diffraction Journal Article Research Support, N.I.H., Extramural Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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