Now showing 1 - 10 of 224
  • 2010Journal Article
    [["dc.bibliographiccitation.firstpage","3036"],["dc.bibliographiccitation.issue","12"],["dc.bibliographiccitation.journal","Inorganica Chimica Acta"],["dc.bibliographiccitation.lastpage","3040"],["dc.bibliographiccitation.volume","363"],["dc.contributor.author","Penkova, Larysa"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Pavlenko, Vadim A."],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.contributor.author","Fritsky, Igor O."],["dc.date.accessioned","2018-11-07T08:38:00Z"],["dc.date.available","2018-11-07T08:38:00Z"],["dc.date.issued","2010"],["dc.description.abstract","The synthesis, crystal structure and magnetic properties of manganese(III) binuclear complexes [Mn(2)(III)(L-3H)(2)(CH(3)OH)(4)]center dot 2CH(3)OH (1) and [Mn(2)(III)(L-3H)(2)(Py)(4)]center dot 2Py (2) (L = 3-[(1E)-N-hydroxyethanimidoyl]- 4-methyl-1H-pyrazole-5-carboxylic acid) are reported. The ligand contains two distinct donor compartments formed by the pyrazolate-N and the oxime or the carboxylic groups. The complexes were characterized by X-ray single crystal diffraction, revealing that both 1 and 2 consist of dinuclear units in which the two metal ions are linked by double pyrazolate bridges with a planar {Mn(2)N(4)} core. Cryomagnetic measurements show antiferromagnetic interaction with g = 1.99, J = -3.6 cm (1), Theta = -2.02 K for 1 and g = 2.00, J = -3.7 cm (1), Theta = 1.43 K for 2. (C) 2010 Elsevier B. V. All rights reserved."],["dc.identifier.doi","10.1016/j.ica.2010.04.038"],["dc.identifier.isi","000282360200046"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/18673"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Elsevier Science Sa"],["dc.relation.issn","0020-1693"],["dc.title","Binuclear manganese(III) complexes of an unsymmetric pyrazolate-based compartmental ligand with hard donor set"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2021Journal Article
    [["dc.bibliographiccitation.journal","Angewandte Chemie International Edition"],["dc.contributor.author","Li, Ming"],["dc.contributor.author","Gupta, Sandeep K."],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2021-06-01T09:41:09Z"],["dc.date.available","2021-06-01T09:41:09Z"],["dc.date.issued","2021"],["dc.identifier.doi","10.1002/anie.202101387"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/84832"],["dc.language.iso","en"],["dc.notes.intern","DOI-Import GROB-425"],["dc.relation.eissn","1521-3773"],["dc.relation.issn","1433-7851"],["dc.title","Merging Pincer Motifs and Potential Metal–Metal Cooperativity in Cobalt Dinitrogen Chemistry: Efficient Catalytic Silylation of N 2 to N(SiMe 3 ) 3"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]
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  • 2016Journal Article
    [["dc.bibliographiccitation.firstpage","5503"],["dc.bibliographiccitation.issue","17"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","5506"],["dc.bibliographiccitation.volume","138"],["dc.contributor.author","Travieso-Puente, Raquel"],["dc.contributor.author","Broekman, J. O. P."],["dc.contributor.author","Chang, Mu-Chieh"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Meyer, Franc"],["dc.contributor.author","Otten, Edwin"],["dc.date.accessioned","2018-11-07T10:14:26Z"],["dc.date.available","2018-11-07T10:14:26Z"],["dc.date.issued","2016"],["dc.description.abstract","Spin-crossover in a pseudo-tetrahedral bis(formazanate) iron(II) complex (1) is described. Structural, magnetic, and spectroscopic analyses indicate that this compound undergoes thermal switching between an S=0 and an S=2 state, which is very rare in four-coordinate complexes. The transition to the high-spin state is accompanied by an increase in Fe-N bond lengths and a concomitant contraction of intraligand N-N bonds. The latter suggests that stabilization of the low-spin state is due to the pi-acceptor properties of the ligand. One-electron reduction of 1 leads to the formation of the corresponding anion, which contains a low-spin (S=1/2) Fe(I) center. The findings are rationalized by electronic structure calculations using density functional theory."],["dc.identifier.doi","10.1021/jacs.6b01552"],["dc.identifier.isi","000375521100008"],["dc.identifier.pmid","27074728"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/40618"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0002-7863"],["dc.title","Spin-Crossover in a Pseudo-tetrahedral Bis(formazanate) Iron Complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2014Journal Article
    [["dc.bibliographiccitation.firstpage","7428"],["dc.bibliographiccitation.issue","20"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","7434"],["dc.bibliographiccitation.volume","136"],["dc.contributor.author","Dalle, Kristian"],["dc.contributor.author","Gruene, Tim"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T09:40:02Z"],["dc.date.available","2018-11-07T09:40:02Z"],["dc.date.issued","2014"],["dc.description.abstract","The ability of many copper metalloenzymes to activate 02 and transfer it to organic substrates has motivated extensive attention in the literature. Investigations focusing on synthetic analogues have provided a detailed understanding of the structures of potential intermediates, thereby helping to guide mechanistic studies. We report herein a crystallographically characterized synthetic Cu-2(II)(mu-eta(1):eta(1)-O-2) complex exhibiting cis-peroxo bonding geometry, known in iron chemistry but previously unobserved for copper. Detailed investigation by UV-vis, resonance Raman, and infrared spectroscopies provides evidence for a significantly diminished copper-oxygen interaction (epsilon approximate to 3000 M-1 cm(-1), nu(Cu-O) = 437 cm(-1), nu(O-O) = 799 cm(-1)) relative to those in known 'coupled' Cu2O2 species, consistent with magnetic measurements which show that the peroxide mediates only weak antiferromagnetic coupling (-2J = 144 cm(-1)). These characteristics are comparable with those of a computationally predicted transition state for 02 binding to type 3 copper centers, providing experimental evidence for the proposed mechanism of O-2 activation and supporting the biological relevance of the Cu-2(II)(mu-eta(1):eta(1)-O-2) cis-species. The peroxide bonding arrangement also allows binding of sodium cations, observed both in the solid state and in solution. Binding induces changes on an electronic level, as monitored by UV-vis spectroscopy (K-a = 1700 M-1), reminiscent of redox-inactive metal binding by iron-oxygen species. The results presented highlight the analogous chemistry these reactive oxygen species undergo, with respect to both their mechanism of formation, and the molecular interactions in which they participate."],["dc.identifier.doi","10.1021/ja5025047"],["dc.identifier.isi","000336416600038"],["dc.identifier.pmid","24766458"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/33423"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0002-7863"],["dc.title","Weakly Coupled Biologically Relevant Cu-2(II)(mu-eta(1):eta(1)-O-2) cis-Peroxo Adduct that Binds Side-On to Additional Metal Ions"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2016Journal Article
    [["dc.bibliographiccitation.firstpage","8088"],["dc.bibliographiccitation.issue","21"],["dc.bibliographiccitation.journal","Macromolecules"],["dc.bibliographiccitation.lastpage","8097"],["dc.bibliographiccitation.volume","49"],["dc.contributor.author","Smolne, Sebastian"],["dc.contributor.author","Buback, Michael"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Matyjaszewsk, Krzysztof"],["dc.contributor.author","Meyer, Franc"],["dc.contributor.author","Schroeder, Hendrik"],["dc.contributor.author","Simakova, Antonina"],["dc.date.accessioned","2018-11-07T10:05:51Z"],["dc.date.available","2018-11-07T10:05:51Z"],["dc.date.issued","2016"],["dc.description.abstract","A speciation analysis for Fe-mesohemin-(MPEG(500))(2)-mediated reversible-deactivation radical polymerization (RDRP) in aqueous solution was carried out by a combination of visible (vis) and Fe-57 Mossbauer spectroscopy. The results were used within kinetic studies of ATRP and OMRP reactions via highly time-resolved EPR spectroscopy. ATRP control was effective with the rate coefficient for deactivation clearly exceeding the one for formation of organometallic species. Deactivation rate coefficients increase by more than 1 order of magnitude in passing from polymerization in 30 to 90 wt % H2O. Media with water contents of and above 70 wt % are well suited for controlled ATRP. The Fe-mesohemin catalyst provides an exceptionally high ATRP equilibrium constant even at ambient temperature, which approaches the one of highly active Cu catalysts."],["dc.identifier.doi","10.1021/acs.macromol.6b01774"],["dc.identifier.isi","000387519200006"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/38983"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1520-5835"],["dc.relation.issn","0024-9297"],["dc.title","Kinetics of Fe-Mesohemin-(MPEG(500))(2)-Mediated RDRP in Aqueous Solution"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2014Journal Article
    [["dc.bibliographiccitation.firstpage","806"],["dc.bibliographiccitation.issue","2"],["dc.bibliographiccitation.journal","Dalton Transactions"],["dc.bibliographiccitation.lastpage","816"],["dc.bibliographiccitation.volume","43"],["dc.contributor.author","Falkenhagen, Jan P."],["dc.contributor.author","Limberg, Christian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Horn, Sebastian"],["dc.contributor.author","Haumann, Michael"],["dc.contributor.author","Braun, Beatrice"],["dc.contributor.author","Mebs, Stefan"],["dc.date.accessioned","2018-11-07T09:47:16Z"],["dc.date.available","2018-11-07T09:47:16Z"],["dc.date.issued","2014"],["dc.description.abstract","The reaction between [(TPA) Fe(MeCN)(2)](OTf)(2) and [nBu(4)N](Cp MoO3) yields the novel tetranuclear complex [(TPA) Fe(mu-Cp MoO3)](2)(OTf)(2), 1, with a rectangular [Mo-O-Fe-O-](2) core containing high-spin iron(II) centres. 1 proved to be an efficient initiator/(pre)catalyst for the autoxidation of cis-cyclooctene with O-2 to give cyclooctene epoxide. To test, which features of 1 are essential in this regard, analogues with zinc(II) and cobalt(II) central atoms, namely [(TPA)Zn(Cp MoO3)](OTf), 3, and [(TPA) Co(Cp MoO3)](OTf), 4, were prepared, which proved to be inactive. The precursor compounds of 1, [(TPA) Fe(MeCN)(2)](OTf)(2) and [nBu(4)N](Cp MoO3) as well as Cp-2 Mo2O5, were found to be inactive, too. Reactivity studies in the absence of cyclooctene revealed that 1 reacts both with O-2 and PhIO via loss of the Cp ligands to give the triflate salt 2 of the known cation [((TPA)Fe)(2)(mu-O)(mu-MoO4)](2+). The cobalt analogue 4 reacts with O-2 in a different way yielding [((TPA)Co)(2)(mu-Mo2O8)](OTf)(2), 5, featuring a Mo2O84- structural unit which is novel in coordination chemistry. The compound [(TPA) Fe(mu-MoO4)](2), 6, being related to 1, but lacking Cp ligands failed to trigger autoxidation of cyclooctene. However, initiation of autoxidation by Cp radicals was excluded via experiments including thermal dissociation of Cp-2 ."],["dc.identifier.doi","10.1039/c3dt52349g"],["dc.identifier.isi","000327894400052"],["dc.identifier.pmid","24154868"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/35073"],["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.title","Iron-molybdenum-oxo complexes as initiators for olefin autoxidation with O-2"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2012Journal Article
    [["dc.bibliographiccitation.firstpage","8141"],["dc.bibliographiccitation.issue","15"],["dc.bibliographiccitation.journal","Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","8149"],["dc.bibliographiccitation.volume","51"],["dc.contributor.author","Das, Animesh"],["dc.contributor.author","Klinke, Felix J."],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Meyer, Steffen"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T09:07:18Z"],["dc.date.available","2018-11-07T09:07:18Z"],["dc.date.issued","2012"],["dc.description.abstract","A new family of tetranuclear nickel cube complexes [Ni4L4(solv)(4)} (1, solv = MeOH; 2, solv = H2O; H2L = pyrazole-based tridentate {ONO} ligand) has been studied in detail, in particular by X-ray diffraction and superconducting quantum interference device (SQUID) magnetometry. Different solvates 1 center dot H2O, 2 center dot 4C(3)H(6)O, 2-CH2Cl2, and 2 center dot H2O were obtained in crystalline form. Only small structural variations were found for the Ni-O-Ni angles of the [Ni4O4] cores of those compounds, but these slight variations have dramatic consequences for the magnetic properties. [Ni4L4(MeOH)(4)}center dot H2O (1 center dot H2O) and [Ni4L4(H2O)(4)]center dot H2O (2 center dot H2O) can be reversibly interconverted in the solid state by exposure to the respective solvent, MeOH or H2O, and this goes along with a switching of the spin ground state from magnetic (S-T = 4) to diamagnetic (S-T = 0). Likewise the (irreversible) loss of lattice solvent in [Ni4L4(H2O)(4)]center dot 4C(3)H(6)O (2 center dot 4C(3)H(6)O) to give 2 center dot 2C(3)H(6)O changes the ground state from S-T = 4 to S-T = 0. In view of these dramatic solvatomagnetic effects for the present [Ni4L4(solv)(4)] complexes, which occur upon extrusion of lattice solvent or facile exchange of coordinated solvent molecules while keeping the robust [Ni4O4] core intact, a note of care is issued: whenever magnetic data are obtained for powdered material or for crystals that easily loose lattice solvent molecules, the magnetic properties may not necessarily reflect the situation observed in the corresponding single crystal diffraction study. Finally, a thorough analysis of the present series of complexes as well as other {Ni-4(mu(3)-OR)(4)} cubes reported in the literature confirms that a correlation between the (Ni-O-Ni)(av) bond angle and J in {Ni4O4} cubane complexes does indeed exist."],["dc.description.sponsorship","DFG [SFB 602]"],["dc.identifier.doi","10.1021/ic300535d"],["dc.identifier.isi","000307134700026"],["dc.identifier.pmid","22823896"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/25763"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0020-1669"],["dc.title","Reversible Solvatomagnetic Effect in Novel Tetranuclear Cubane-Type Ni-4 Complexes and Magnetostructural Correlations for the [Ni-4(mu(3)-O)(4)] Core"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2018Journal Article
    [["dc.bibliographiccitation.firstpage","1862"],["dc.bibliographiccitation.issue","13"],["dc.bibliographiccitation.journal","CrystEngComm"],["dc.bibliographiccitation.lastpage","1873"],["dc.bibliographiccitation.volume","20"],["dc.contributor.author","Molčanov, Krešimir"],["dc.contributor.author","Stalke, Dietmar"],["dc.contributor.author","Šantić, Ana"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Stilinović, Vladimir"],["dc.contributor.author","Mou, Zhongyu"],["dc.contributor.author","Kertesz, Miklos"],["dc.contributor.author","Kojić-Prodić, Biserka"],["dc.date.accessioned","2020-12-10T18:11:15Z"],["dc.date.available","2020-12-10T18:11:15Z"],["dc.date.issued","2018"],["dc.identifier.doi","10.1039/C7CE02146A"],["dc.identifier.eissn","1466-8033"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/73937"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.title","Probing semiconductivity in crystals of stable semiquinone radicals: organic salts of 5,6-dichloro-2,3-dicyanosemiquinone (DDQ) radical anions"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]
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  • 2015Journal Article
    [["dc.bibliographiccitation.firstpage","4670"],["dc.bibliographiccitation.issue","14"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","4673"],["dc.bibliographiccitation.volume","137"],["dc.contributor.author","Roy, Sudipta"],["dc.contributor.author","Stueckl, A. Claudia"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Dittrich, Birger"],["dc.contributor.author","Meyer, Jann"],["dc.contributor.author","Maity, Bholanath"],["dc.contributor.author","Koley, Debasis"],["dc.contributor.author","Schwederski, Brigitte"],["dc.contributor.author","Kaim, Wolfgang"],["dc.contributor.author","Roesky, Herbert W."],["dc.date.accessioned","2018-11-07T09:58:29Z"],["dc.date.available","2018-11-07T09:58:29Z"],["dc.date.issued","2015"],["dc.description.abstract","Intermediate species dichlorosilylene was generated in situ from trichlorosilane and inserted into the P-Cl bond of diphenylchlorophosphine (Ph2P-Cl) to obtain Ph2P-SiCl3 (1). Monodechlorination of 1 by cyclic alkyl(amino) carbenes (cAACs)/KC8 in THF at low temperature led to the formation of stable radicals Ph2P-Si(cAAC)Cl-2 (2a,b). Compounds 2a,b were characterized by X-ray single crystal diffraction, mass spectrometry and studied by cyclic voltammetry and theoretical calculations. Radical properties of 2 are confirmed by EPR measurements that suggest the radical electron in 2 couples with N-14 (I = 1), Cl-35/37 (I = 3/2), and P-31 (I = 1/2) nuclei leading to multiple hyperfine lines. Hyperfine coupling parameters computed from DFT calculations are in good agreement with those of experimental values. Electronic distributions obtained from the theoretical calculations suggest that the radical electron mostly resides on the carbene C of 2."],["dc.identifier.doi","10.1021/jacs.5b02403"],["dc.identifier.isi","000353177100020"],["dc.identifier.pmid","25815606"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/37370"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0002-7863"],["dc.title","Stable Radicals from Commonly Used Precursors Trichlorosilane and Diphenylchlorophosphine"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]
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  • 2013Journal Article
    [["dc.bibliographiccitation.firstpage","10101"],["dc.bibliographiccitation.issue","31"],["dc.bibliographiccitation.journal","Chemistry - A European Journal"],["dc.bibliographiccitation.lastpage","10106"],["dc.bibliographiccitation.volume","19"],["dc.contributor.author","Albers, Antonia"],["dc.contributor.author","Bayer, Thomas A."],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T09:22:18Z"],["dc.date.available","2018-11-07T09:22:18Z"],["dc.date.issued","2013"],["dc.description.sponsorship","DFG [IGRK 1422]; Cusanuswerk"],["dc.identifier.doi","10.1002/chem.201301760"],["dc.identifier.isi","000321983700006"],["dc.identifier.pmid","23780647"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/29311"],["dc.language.iso","en"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.relation.issn","0947-6539"],["dc.title","A Functional Model for the Rieske Center: Full Characterization of a Biomimetic N-Ligated [2Fe-2S] Cluster in Different Protonation States"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dspace.entity.type","Publication"]]
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