Now showing 1 - 3 of 3
  • 2019Journal Article
    [["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"]]
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  • 2019Journal Article
    [["dc.bibliographiccitation.firstpage","14349"],["dc.bibliographiccitation.issue","40"],["dc.bibliographiccitation.journal","Angewandte Chemie International Edition"],["dc.bibliographiccitation.lastpage","14356"],["dc.bibliographiccitation.volume","58"],["dc.contributor.author","Ghosh, Munmun"],["dc.contributor.author","Cramer, Hanna H."],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Hansmann, Max M."],["dc.contributor.author","Ye, Shengfa"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2019-11-25T10:59:28Z"],["dc.date.accessioned","2021-10-27T13:12:46Z"],["dc.date.available","2019-11-25T10:59:28Z"],["dc.date.available","2021-10-27T13:12:46Z"],["dc.date.issued","2019"],["dc.description.abstract","The reaction of the ferrous complex [LFe(NCMe)2 ](OTf)2 (1), which contains a macrocyclic tetracarbene as ligand (L), with Na(OCP) generates the OCP- -ligated complex [LFe(PCO)(CO)]OTf (2) together with the dinuclear μ-phosphido complex [(LFe)2 P](OTf)3 (3), which features an unprecedented linear Fe-(μ-P)-Fe motif and a \"naked\" P-atom bridge that appears at δ=+1480 ppm in the 31 P NMR spectrum. 3 exhibits rich redox chemistry, and both the singly and doubly oxidized species 4 and 5 could be isolated and fully characterized. X-ray crystallography, spectroscopic studies, in combination with DFT computations provide a comprehensive electronic structure description and show that the Fe-(μ-P)-Fe core is highly covalent and structurally invariant over the series of oxidation states that are formally described as ranging from FeIII FeIII to FeIV FeIV . 3-5 now add a higher homologue set of complexes to the many systems with Fe-(μ-O)-Fe and Fe-(μ-N)-Fe core structures that are prominent in bioinorganic chemistry and catalysis."],["dc.identifier.doi","10.1002/anie.201908213"],["dc.identifier.eissn","1521-3773"],["dc.identifier.isbn","1350785"],["dc.identifier.issn","1433-7851"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16707"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/91720"],["dc.language.iso","en"],["dc.notes.intern","Migrated from goescholar"],["dc.relation.eissn","1521-3773"],["dc.relation.issn","1433-7851"],["dc.relation.orgunit","Fakultät für Chemie"],["dc.rights","CC BY 4.0"],["dc.rights.access","openAccess"],["dc.rights.uri","https://creativecommons.org/licenses/by/4.0"],["dc.subject","N-heterocyclic carbenes; electronic structure; iron complexes; phosphido complexes; redox series"],["dc.subject.ddc","540"],["dc.title","A μ-Phosphido Diiron Dumbbell in Multiple Oxidation States"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2019Journal Article
    [["dc.bibliographiccitation.firstpage","373"],["dc.bibliographiccitation.issue","58"],["dc.bibliographiccitation.journal","Angewandte Chemie. International Edition"],["dc.bibliographiccitation.lastpage","379"],["dc.bibliographiccitation.volume","59"],["dc.contributor.author","Meyer, Andreas"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Dey, Surjendu"],["dc.contributor.author","Höbartner, Claudia"],["dc.contributor.author","Bennati, Marina"],["dc.date.accessioned","2019-12-09T11:04:02Z"],["dc.date.accessioned","2021-10-27T13:12:49Z"],["dc.date.available","2019-12-09T11:04:02Z"],["dc.date.available","2021-10-27T13:12:49Z"],["dc.date.issued","2019"],["dc.description.abstract","Spectroscopic and biophysical methods for structural determination at atomic resolution are fundamental in studies of biological function. Here we introduce an approach to measure molecular distances in bio-macromolecules using 19 F nuclear spins and nitroxide radicals in combination with high-frequency (94 GHz/3.4 T) electron-nuclear double resonance (ENDOR). The small size and large gyromagnetic ratio of the 19 F label enables to access distances up to about 1.5 nm with an accuracy of 0.1-1 Å. The experiment is not limited by the size of the bio-macromolecule. Performance is illustrated on synthesized fluorinated model compounds as well as spin-labelled RNA duplexes. The results demonstrate that our simple but strategic spin-labelling procedure combined with state-of-the-art spectroscopy accesses a distance range crucial to elucidate active sites of nucleic acids or proteins in the solution state."],["dc.identifier.doi","10.1002/anie.201908584"],["dc.identifier.isbn","31539187"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16871"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/91724"],["dc.language.iso","en"],["dc.notes.intern","Migrated from goescholar"],["dc.relation.eissn","1521-3773"],["dc.relation.issn","1521-3773"],["dc.relation.orgunit","Fakultät für Chemie"],["dc.rights","CC BY-NC 4.0"],["dc.rights.access","openAccess"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc/4.0"],["dc.subject","RNA; fluorine; high field ENDOR; spin labelling; structural biology"],["dc.subject.ddc","540"],["dc.title","Measurement of Angstrom to Nanometer Molecular Distances with 19 F Nuclear Spins by EPR/ENDOR Spectroscopy"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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