Demeshko, Serhiy V.

[["dc.bibliographiccitation.firstpage","3866"],["dc.bibliographiccitation.issue","9"],["dc.bibliographiccitation.journal","Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","3887"],["dc.bibliographiccitation.volume","50"],["dc.contributor.author","Jarenmark, Martin"],["dc.contributor.author","Haukka, Matti"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Tuczek, Felix"],["dc.contributor.author","Zuppiroli, Luca"],["dc.contributor.author","Meyer, Franc"],["dc.contributor.author","Nordlander, Ebbe"],["dc.date.accessioned","2018-11-07T08:56:15Z"],["dc.date.available","2018-11-07T08:56:15Z"],["dc.date.issued","2011"],["dc.description.abstract","To model the heterodinuclear active sites in plant purple acid phosphatases, a mononuclear synthon, [Fe(III)(H(2)IPCPMP)(Cl(2))][PF(6)] (1), has been generated in situ from the ligand 2-(N-isopropyl-N-((2-pyridyl)methyDaminomethyl)-6-(N-(carboxylmethyl)-N-((2-pyridyl)methyl)amino-methyl) -4methylphenol (IPCPMP) and used to synthesize heterodinudear complexes of the formulas [Fe(III)M(II)(IPCPMP)(OAc)(2)(CH(3)OH)][PF(6)] (M = Zn (2), Co (3), Ni (4), Mn (5)), [Fe(III)Zn(II)(IPCPMP)(mpdp)][PF(6)] (6) (mpdp = meta-phenylene-dipropionate), and [Fe(III)Cu(II)(IPCPMP) (OAc))(2)(mu-O)][PF(6)] (7). Complexes 2-4, 6, and 7 have been crystallographically characterized. The structure of 6 is a solid state coordination polymer with heterodinuclear monomeric units, and 7 is a tetranuclear complex consisting of two heterodinuclear phenolate-bridged Fe(III)Cu(II) units bridged through a it-oxido group between the two Fe(III) ions. Mossbauer spectra confirm the presence of high spin Fe(III) in an octahedral environment for 1, 3, and 5 while 2 and 4 display relaxation effects. Magnetic susceptibility measurements indicate weak antiferromagnetic coupling for 3, 4, and 5 and confirm the assignment of the metal centers in 2-5 as high spin Fe(III)-M(II) (M = Zn, Co (high spin), Ni (high spin), Mn (high spin)). Complexes 2-5 are intact in acetonitrile solution as indicated by IR spectroscopy (for 2-4) and electrospray ionization mass spectrometry (ESI-MS) but partly dissociate to hydroxide species and a mononuclear complex in water/acetonitrile solutions. UV-vis spectroscopy reveal pH-dependent behavior, and species that form upon increasing the pH have been assigned to mu-hydroxido-bridged Fe(III)M(II) complexes for 2-5 although 2 and 3 is further transformed into what is propsed to be a mu-oxido-bridged tetranuclear complex similar to 7. Complexes 2-5 enhance phosphodiester cleavage of 2-hydroxy-propyl-p-nitrophenyl phosphate (HPNP) and bis(2,4-dinitrophenyl)phosphate (BDNPP), but the reactivities are different for different complexes and generally show strong pH dependence."],["dc.description.sponsorship","Swedish Research Council (VR); Royal Physiographic Society"],["dc.identifier.doi","10.1021/ic1020324"],["dc.identifier.isi","000289710700006"],["dc.identifier.pmid","21452875"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/9428"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/23098"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0020-1669"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Synthesis, Characterization, and Reactivity Studies of Heterodinuclear Complexes Modeling Active Sites in Purple Acid Phospatases"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","13289"],["dc.bibliographiccitation.issue","34"],["dc.bibliographiccitation.journal","Dalton Transactions"],["dc.bibliographiccitation.lastpage","13293"],["dc.bibliographiccitation.volume","45"],["dc.contributor.author","Das, Biswanath"],["dc.contributor.author","Lee, Bao-Lin"],["dc.contributor.author","Karlsson, Erik A."],["dc.contributor.author","Akermark, Torbjorn"],["dc.contributor.author","Shatskiy, Andrey"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Liao, Rong-Zhen"],["dc.contributor.author","Laine, Tanja M."],["dc.contributor.author","Haukka, Matti"],["dc.contributor.author","Zeglio, Erica"],["dc.contributor.author","Abdel-Magied, Ahmed F."],["dc.contributor.author","Siegbahn, Per E. M."],["dc.contributor.author","Meyer, Franc"],["dc.contributor.author","Karkas, Markus D."],["dc.contributor.author","Johnston, Eric V."],["dc.contributor.author","Nordlander, Ebbe"],["dc.contributor.author","Akermark, Bjorn"],["dc.date.accessioned","2018-11-07T10:08:33Z"],["dc.date.available","2018-11-07T10:08:33Z"],["dc.date.issued","2016"],["dc.description.abstract","The synthesis of two molecular iron complexes, a dinuclear iron(III,III) complex and a nonanuclear iron complex, based on the di-nucleating ligand 2,2'-(2-hydroxy-5-methyl-1,3-phenylene)bis(1H-benzo[d]imidazole-4-carboxylic acid) is described. The two iron complexes were found to drive the oxidation of water by the one-electron oxidant [Ru(bpy)(3)](3+)."],["dc.identifier.doi","10.1039/c6dt01554a"],["dc.identifier.isi","000382144300004"],["dc.identifier.pmid","27265239"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/13417"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/39484"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1477-9234"],["dc.relation.issn","1477-9226"],["dc.rights","CC BY-NC 3.0"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc/3.0"],["dc.title","Water oxidation catalyzed by molecular di- and nonanuclear Fe complexes: importance of a proper ligand framework"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","97"],["dc.bibliographiccitation.journal","Frontiers in Chemistry"],["dc.bibliographiccitation.lastpage","97"],["dc.bibliographiccitation.volume","7"],["dc.contributor.author","Das, Biswanath"],["dc.contributor.author","Al-Hunaiti, Afnan"],["dc.contributor.author","Sánchez-Eguía, Brenda N."],["dc.contributor.author","Zeglio, Erica"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Braunger, Steffen"],["dc.contributor.author","Haukka, Matti"],["dc.contributor.author","Repo, Timo"],["dc.contributor.author","Castillo, Ivan"],["dc.contributor.author","Nordlander, Ebbe"],["dc.date.accessioned","2019-07-09T11:50:31Z"],["dc.date.available","2019-07-09T11:50:31Z"],["dc.date.issued","2019"],["dc.description.abstract","The new di- and tetranuclear Fe(III) μ-oxido complexes [Fe4(μ-O)4(PTEBIA)4](CF3SO3)4(CH3CN)2] (1a), [Fe2(μ-O)Cl2(PTEBIA)2](CF3SO3)2 (1b), and [Fe2(μ-O)(HCOO)2(PTEBIA)2](ClO4)2 (MeOH) (2) were prepared from the sulfur-containing ligand (2-((2,4-dimethylphenyl)thio)-N,N-bis ((1-methyl-benzimidazol-2-yl)methyl)ethanamine (PTEBIA). The tetrairon complex 1a features four μ-oxido bridges, while in dinuclear 1b, the sulfur moiety of the ligand occupies one of the six coordination sites of each Fe(III) ion with a long Fe-S distance of 2.814(6) Å. In 2, two Fe(III) centers are bridged by one oxido and two formate units, the latter likely formed by methanol oxidation. Complexes 1a and 1b show broad sulfur-to-iron charge transfer bands around 400-430 nm at room temperature, consistent with mononuclear structures featuring Fe-S interactions. In contrast, acetonitrile solutions of 2 display a sulfur-to-iron charge transfer band only at low temperature (228 K) upon addition of H2O2/CH3COOH, with an absorption maximum at 410 nm. Homogeneous oxidative catalytic activity was observed for 1a and 1b using H2O2 as oxidant, but with low product selectivity. High valent iron-oxo intermediates could not be detected by UV-vis spectroscopy or ESI mass spectrometry. Rather, evidence suggest preferential ligand oxidation, in line with the relatively low selectivity and catalytic activity observed in the reactions."],["dc.identifier.doi","10.3389/fchem.2019.00097"],["dc.identifier.pmid","30881952"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/15951"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/59784"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.relation.issn","2296-2646"],["dc.rights","CC BY 4.0"],["dc.rights.uri","https://creativecommons.org/licenses/by/4.0"],["dc.subject.ddc","540"],["dc.title","Di- and Tetrairon(III) μ-Oxido Complexes of an N3S-Donor Ligand: Catalyst Precursors for Alkene Oxidations"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]