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Dechert, Sebastian
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Dechert, Sebastian
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Dechert, Sebastian
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Dechert, S.
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7003844285
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2009Journal Article [["dc.bibliographiccitation.firstpage","10049"],["dc.bibliographiccitation.issue","21"],["dc.bibliographiccitation.journal","Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","10059"],["dc.bibliographiccitation.volume","48"],["dc.contributor.author","Stollenz, Michael"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Gehring, Henrike"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Grosse, Christian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T11:22:18Z"],["dc.date.available","2018-11-07T11:22:18Z"],["dc.date.issued","2009"],["dc.description.abstract","The synthesis of three pyrazole-based, potentially binucleating ligands 3,5-bis(R(1)N(CH(3))CH(2))-4-R(2)pyrazole (L(1)H: R(1) pyridyl-2-methyl-, R(2) = Ph; L(2)H: R(1) = 8-quinolyl-, R(2) = H; L(3)H: R(1) = 8-quinolyl-, R(2) = Ph) is described. Reaction of L(1-3)H with 1 equiv. of mesitylcopper affords oligonuclear homoleptic complexes of the type [CuL](n) (1-3). The single crystal X-ray structure of 2 shows a tetranuclear assembly of linear coordinated copper(I)-centers bridged by pyrazolato ligands that alternate above and below the Cu(4) plane, with additional weak interactions from some of the ligand side arms. As the single crystal X-ray structure of 3 reveals, phenyl substitution at the 4-position of the pyrazolato framework leads to significant structural modification of the Cu(4) array, giving a rhombical tetranuclear complex with two linear coordinated copper(I) centers that exhibit a short intramolecular Cu:: center dot Cu contact (2.8212(10) angstrom) and two peripheral copper(I) centers in a distorted tetrahedral coordination mode. Thus, 3 represents a very rare example of an inorganic pyrazolato cuprate which can also be viewed as a partly rearranged structural isomer of 2. Furthermore, the crystal lattice of 3 shows an extended network of intra- and intermolecular pi-pi stacking interactions between the aromatic rings. In solution, 1-3 each form two types of oligomers a and b that slowly (<1 s(-1)) equilibrate at room temperature. Using Diffusion Ordered Spectroscopy (DOSY) and variable temperature (1)H NMR spectroscopy it can be shown that a and b correspond to a tetrameric and a (planar) trimeric species. Coordination of the pyridyl/quinolyl side arms that is observed in the solid state seems to be only transient in solution."],["dc.description.sponsorship","Fonds der Chernischen Industrie"],["dc.identifier.doi","10.1021/ic900727h"],["dc.identifier.isi","000270987400019"],["dc.identifier.pmid","19803532"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/55964"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0020-1669"],["dc.title","Oligonuclear Homoleptic Copper(I) Pyralzolates with Multinucleating Ligand Scaffolds: High Structural Diversity in Solid-State and Solution"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI PMID PMC WOS2013Journal Article [["dc.bibliographiccitation.firstpage","796"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","ChemCatChem"],["dc.bibliographiccitation.lastpage","805"],["dc.bibliographiccitation.volume","5"],["dc.contributor.author","Saha, Tapan Kumar"],["dc.contributor.author","Frauendorf, Holm"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T09:27:35Z"],["dc.date.available","2018-11-07T09:27:35Z"],["dc.date.issued","2013"],["dc.description.abstract","Dyes in wastewater severely affect the nature and quality of water by inhibiting the sunlight penetration into the stream, which thereby reduces the photosynthesis reaction. This poses a serious environmental threat in many developing countries. Recently, new methods for the treatment of colored dye effluent streams have attracted much attention. The [MnIII(tmpyp)]/H2O2 system (tmpyp=meso-tetrakis(1-methylpyridinium-4-yl)porphyrinato) was now found to degrade various azo dyes with remarkably high efficiency under ambient conditions in aqueous solution at certain pH values. Main products of the catalytic degradation of the dye amaranth by [MnIII(tmpyp)]/H2O2 were analyzed. The reaction mechanism was studied in more detail by using rapid-scan stopped-flow spectrophotometry as a function of pH, [catalyst], [H2O2], [dye], and [surfactants]. Spectral analyses and kinetic data suggested rapid formation of an intermediate [MnIII(tmpyp)(OOH)] (a compound 0-type intermediate), followed by the formation of a relatively stable trans-dioxomanganese(V) porphyrin complex, [MnV(O)2(tmpyp)] (a compoundI analog). The one-electron reduction of [MnV(O)2(tmpyp)] to [MnIV(O)(tmpyp)] (a compoundII analog) was accelerated greatly by amaranth. On the basis of the kinetic and spectroscopic data, a reaction mechanism of the formation of reactive intermediates [MnIII(tmpyp)(OOH)], [MnV(O)2(tmpyp)], and [MnIV(O)(tmpyp)] was proposed."],["dc.description.sponsorship","Alexander von Humboldt Foundation"],["dc.identifier.doi","10.1002/cctc.201200475"],["dc.identifier.isi","000315416200026"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/30572"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Wiley-v C H Verlag Gmbh"],["dc.relation.issn","1867-3880"],["dc.title","Efficient Oxidative Degradation of Azo Dyes by a Water-Soluble Manganese Porphyrin Catalyst"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI WOS2008Journal Article [["dc.bibliographiccitation.firstpage","5146"],["dc.bibliographiccitation.issue","19"],["dc.bibliographiccitation.journal","Organometallics"],["dc.bibliographiccitation.lastpage","5151"],["dc.bibliographiccitation.volume","27"],["dc.contributor.author","Scheele, Ulrich Juergen"],["dc.contributor.author","Georgiou, Maria"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T11:10:05Z"],["dc.date.available","2018-11-07T11:10:05Z"],["dc.date.issued","2008"],["dc.description.abstract","Reaction of Ag2O with the N-heterocyclic carbene (NHC) precursors 3,5-bis[3-(2,4,6-trimethylphenyl)imidazolium-1-ylmethyl]-1H-pyrazole bishexafluorophosphate (1a) and 3,5-bis[3-(2,6-diisopropylphenyl)imidazolium-1-ylmethyl]-1H-pyrazole bishexafluorophosphate (1b) yielded silver(l) complexes 2 and 3, respectively. X-ray crystallography revealed a tetranuclear dimeric solid state structure in the case of 2, whereas an unprecedented octanuclear tetrameric \"double-crown\"-like structure was found for 3, presumably due to the slightly bulkier ligand. Unlike 2, complex 3 is not stable in solution but in equilibrium with tetranuclear and hexanuclear complexes 4 and 5, respectively. The identity of those species could be elucidated by detailed NMR spectroscopic studies (H-1, C-13, N-15, Ag-109, and DOSY experiments), which also provide valuable benchmark data for correlating (1)J(AgN) couplings and Ag-109 chemical shifts with structural information."],["dc.description.sponsorship","Fonds der Chemischen Industrie"],["dc.identifier.doi","10.1021/om800487e"],["dc.identifier.isi","000259604200043"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/53140"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0276-7333"],["dc.title","Combining pyrazolate and N-heterocyclic carbene coordination motifs: Synthesis and characterization of a double-crowned silver complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI WOS2009Journal Article [["dc.bibliographiccitation.firstpage","1542"],["dc.bibliographiccitation.issue","11-12"],["dc.bibliographiccitation.journal","Zeitschrift für Naturforschung B"],["dc.bibliographiccitation.lastpage","1552"],["dc.bibliographiccitation.volume","64"],["dc.contributor.author","Georgiou, Maria"],["dc.contributor.author","Wöckel, Simone"],["dc.contributor.author","Konstanzer, Vera"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2020-11-05T14:37:47Z"],["dc.date.available","2020-11-05T14:37:47Z"],["dc.date.issued","2009"],["dc.description.abstract","A set of pyrazole-bridged bis(imidazolium) compounds [H(3)L(1)]X(2) - [H(3)L(4)]X(2) (L(1) = 3,5-bis[1-(tert-butyl)imidazolium-1-ylmethyl]-1H-pyrazole; L(2) = 3,5-bis[1-(tert-butyl)imidazolium-1-ylmethyl]-4-phenyl-1H-pyrazole; L(3) = 3,5-bis[1-(1-adamantyl)imidazolium-1-ylmethyl]-1H-pyrazole; L(4) = 3,5-bis[1-(1-adamantyl)imidazolium-1-ylmethyl]-4-phenyl-1H-pyrazole; X = Cl(-). BF(4)(-) or PF(6)(-)) has been prepared, and three compounds have been characterized by X-ray crystallography. The unique [H(3)L(4)][H(2)L(4)](PF(6))(3) features a dimeric face-to-face arrangement of two molecules due to the involvement of both the pyrazole-NH and the imidazolium C(2)H in hydrogen bonding. [H(3)L(1)]X(2) - [H(3)L(4)]X(2) serve as precursors for silver(I) complexes with compartmental pyrazolate-bridged bis(NHC) ligands. The complexes have been readily prepared by the Ag(2)O route and feature either the known [(L(1-4))(2)Ag(4)](2+) or the new [(H(2)L(1))(4)Ag(4)](8+) motif, depending on the solvent for the reaction (MeCN or acetone). [(H(2)L(1))(4)Ag(4)](PF(6))(8) contains a central (pzAg)(4) ring with pendant imidazolium side arms. Upon further reaction with Ag(2)O in MeCN it was found to undergo transformation to the corresponding [(L(1))(2)Ag(4)](PF(6))(2). All complexes have been thoroughly studied by NMR spectroscopy in solution, and preliminary luminescence data of [(H(2)L(1))(4)Ag(4)](PF(6))(8) have been recorded."],["dc.identifier.doi","10.1515/znb-2009-11-1238"],["dc.identifier.isi","000273712900038"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/68196"],["dc.notes.intern","DOI Import GROB-352"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Verlag Z Naturforsch"],["dc.relation.eissn","1865-7117"],["dc.relation.issn","0932-0776"],["dc.title","Structural Variations in Tetrasilver(I) Complexes of Pyrazolate-bridged Compartmental N-Heterocyclic Carbene Ligands"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI WOS2019Journal Article [["dc.bibliographiccitation.journal","Angewandte Chemie"],["dc.contributor.author","Meyer, Franc"],["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.date.accessioned","2019-08-05T10:02:30Z"],["dc.date.available","2019-08-05T10:02:30Z"],["dc.date.issued","2019"],["dc.description.abstract","Reaction of the ferrous complex [LFe(NCMe)2](OTf)2 (1) containing a macrocyclic tetracarbene as ligand with Na(OCP) generates OCP− ligated complex [LFe(PCO)(CO)]OTf (2) together with dinuclear μ‐phosphido complex [(LFe)2P](OTf)3 (3) featuring an unprecedented linear Fe‐(μ‐P)‐Fe motif and a \"naked\" P‐atom bridge that appears at +1480 ppm in the 31P NMR spectrum. 3 is shown to exhibit rich redox chemistry, and both singly and doubly oxidized species 4 and 5 could be isolated and fully characterized. X‐ray crystallography, UV‐vis, EPR and 57Fe Mößbauer spectroscopies in combination with DFT computations provide a comprehensive electronic structure description and evidence 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 FeIIIFeIII to FeIVFeIV. 3 – 5 now add a higher homologue set of complexes to 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/ange.201908213"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/62277"],["dc.language.iso","en"],["dc.relation.issn","0044-8249"],["dc.relation.issn","1521-3757"],["dc.title","A µ‐Phosphido Diiron Dumbbell in Multiple Oxidation States"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]Details DOI2009Journal Article [["dc.bibliographiccitation.firstpage","90"],["dc.bibliographiccitation.issue","1"],["dc.bibliographiccitation.journal","Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","99"],["dc.bibliographiccitation.volume","48"],["dc.contributor.author","Ballmann, Joachim"],["dc.contributor.author","Fuchs, Michael G. G."],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T08:33:35Z"],["dc.date.available","2018-11-07T08:33:35Z"],["dc.date.issued","2009"],["dc.description.abstract","Chelating 3,3'-R(1)-5,5'-R(2) -2,2'-dithiobiphenyl ligands (R(1) = R(2) = Cl, 4a; R(1) = R(2) = (t)Bu, 4b; R(1) = allyl, R(2) = H, 4c) and the 2,2'-methylenedibenzenethiol ligand (4d) were synthesized from the corresponding diols (1a-1d) via a three-step procedure involving a Miyazaki-Newman-Kwart rearrangement. Zinc complexes and a tin complex (for 4c) have been prepared to explore their coordination potential, and the substitution pattern, as well as the chelate ring size, is shown to severely effect their ligating properties. Four of the complexes have been characterized crystallographically in the solid state, and the nuclearity of the zinc complexes in solution has been studied by diffusion-ordered NMR spectroscopy. Depending on the ligand, zinc complexes [(4)Zn(4,4'-(t)Bu-bipyridine)](n) (5a-d) are monomeric (n = 1; 4b, 4c), monomeric in solution and dimeric in the solid state (n = 1, 2; 4a), or dimeric overall (n = 2; 4d). The tin complex (4c)SnPh(2) (6c) was additionally synthesized to prove the coordinating abilities of the allyl substituted ligand 4c."],["dc.description.sponsorship","DFG; Fonds der Chemischen Industrie"],["dc.identifier.doi","10.1021/ic801285u"],["dc.identifier.isi","000262011700016"],["dc.identifier.pmid","19035679"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/17611"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0020-1669"],["dc.title","Synthesis and Coordination Properties of Chelating Dithiophenolate Ligands"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI PMID PMC WOS2008Journal Article [["dc.bibliographiccitation.firstpage","373"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","European Journal of Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","377"],["dc.contributor.author","Scheele, Ulrich Juergen"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T11:19:51Z"],["dc.date.available","2018-11-07T11:19:51Z"],["dc.date.issued","2008"],["dc.description.abstract","A set of compartmental pyrazole-based ligands with appended NHC donors has been synthesized and isolated as [H4L]Cl-3 and [H3L](PF6)(2) salts. Dinuclear (allyl)palladium complexes of these ligands are conveniently accessible via the in situ prepared silver species. Three complexes [(allyl)(2)Pd2L]PF6 and one derivative [(methallyl)(2)Pd2L]PF6 have been characterized crystallographically, which revealed that the metal ions are positioned in close proximity [d(Pd center dot center dot center dot Pd) = 3.97-4.05 angstrom], with two possible mutual orientations of the (meth)allyl ligands within the dimetallic pocket. NMR spectroscopy shows slow interconversion of these isomers (k = 0.05-0.4 s(-1)), where the (meth)allyl ligands are detached trans to the carbene during this eta(3)-eta(1)-eta(3) dynamic process. ((C) Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)."],["dc.identifier.doi","10.1002/ejic.200701230"],["dc.identifier.isi","000253044800003"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/55386"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Wiley-v C H Verlag Gmbh"],["dc.relation.issn","1434-1948"],["dc.title","Pyrazole-bridged NHC ligands and their dimetallic (allyl)palladium complexes"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI WOS2016Journal Article [["dc.bibliographiccitation.firstpage","2307"],["dc.bibliographiccitation.issue","7"],["dc.bibliographiccitation.journal","Chemistry - A European Journal"],["dc.bibliographiccitation.lastpage","2316"],["dc.bibliographiccitation.volume","22"],["dc.contributor.author","Vogel, Anastasia"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Brueckner, Christian"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T10:18:14Z"],["dc.date.available","2018-11-07T10:18:14Z"],["dc.date.issued","2016"],["dc.description.abstract","Oxidation of a nonaromatic Siamese-twin porphyrin, a pyrazole-containing expanded porphyrin with two porphyrinlike binding pockets, with a stoichiometric amount of the two-electron, two-proton oxidizing agent 2,3-dichloro-5,6-dicyano-1,4-benzochinone led to the formation of a single N-pz-Co-Ph linkage between the pyrazole unit with a neighboring meso-phenyl group, forming a pyrazolo- [1,5-a]indole moiety. Repeated treatment with a second equivalent of the oxidant yielded a doubly N-fused species, involving the second pyrazole moiety. The conversion products were characterized by variable-temperature and multinuclear 1D and 2DNMR spectroscopy. The fusions strongly alter the conformation of the macrocycles, as shown by X-ray diffraction analyses of all three compounds, eventually leading to a folded structure. UV/Vis and NMR-spectroscopic investigations indicated the presence of highly delocalized but nonmacrocycle-aromatic systems. This behavior of the Siamese-twin porphyrin in response to oxidation is in contrast to the behavior of related all-pyrrole-based expanded macrocycles that switch, by redox processes and protonation, between Huckel and Mobius aromatic states."],["dc.description.sponsorship","Studienstiftung des deutschen Volkes; NSF [CHE-1058846]"],["dc.identifier.doi","10.1002/chem.201503699"],["dc.identifier.isi","000369855000017"],["dc.identifier.pmid","26670580"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/41396"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Wiley-v C H Verlag Gmbh"],["dc.relation.issn","1521-3765"],["dc.relation.issn","0947-6539"],["dc.title","Siamese-Twin Porphyrin Origami: Oxidative Fusing and Folding"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]Details DOI PMID PMC WOS2017Journal Article [["dc.bibliographiccitation.firstpage","16720"],["dc.bibliographiccitation.issue","46"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","16731"],["dc.bibliographiccitation.volume","139"],["dc.contributor.author","Manz, Dennis-Helmut"],["dc.contributor.author","Duan, Peng-Cheng"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Oswald, Rainer"],["dc.contributor.author","John, Michael"],["dc.contributor.author","Mata, Ricardo A."],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2019-08-05T09:50:28Z"],["dc.date.accessioned","2020-05-12T10:19:16Z"],["dc.date.available","2019-08-05T09:50:28Z"],["dc.date.available","2020-05-12T10:19:16Z"],["dc.date.issued","2017"],["dc.description.abstract","A compartmental ligand scaffold HL with two β-diketiminato binding sites spanned by a pyrazolate bridge gave a series of dinuclear nickel(II) dihydride complexes M[LNi2(H)2], M = Na (Na·2) and K (K·2), which were isolated after reacting the precursor complex [LNi2(μ-Br)] (1) with MHBEt3 (M = Na and K). Crystallographic characterization showed the two hydride ligands to be directed into the bimetallic pocket, closely interacting with the alkali metal cation. Treatment of K·2 with dibenzo(18-crown-6) led to the separated ion pair [LNi2(H)2][K(DB18C6)] (2[K(DB18C6)]). Reaction of Na·2 or K·2 with D2 was investigated by a suite of 1H and 2H NMR experiments, revealing an unusual pairwise H2/D2 exchange process that synchronously involves both Ni-H moieties without H/D scrambling. A mechanistic picture was provided by DFT calculations which suggested facile recombination of the two terminal hydrides within the bimetallic cleft, with a moderate enthalpic barrier of ∼62 kJ/mol, to give H2 and an antiferromagnetically coupled [LNiI2]- species. This was confirmed by SQUID monitoring during H2 release from solid 2[K(DB18C6)]. Interaction with the Lewis acid cation (Na+ or K+) significantly stabilizes the dihydride core. Kinetic data for the M[L(Ni-H)2] → H2 transition derived from 2D 1H EXSY spectra confirmed first-order dependence of H2 release on M·2 concentration and a strong effect of the alkali metal cation M+. Treating [LNi2(D)2]- with phenylacetylene led to D2 and dinickel(II) complex 3- with a twice reduced styrene-1,2-diyl bridging unit in the bimetallic pocket. Complexes [LNiII2(H)2]- having two adjacent terminal hydrides thus represent a masked version of a highly reactive dinickel(I) core. Storing two reducing equivalents in adjacent metal hydrides that evolve H2 upon substrate binding is reminiscent of the proposed N2 binding step at the FeMo cofactor of nitrogenase, suggesting the use of the present bimetallic scaffold for reductive bioinspired activation of a range of inert small molecules."],["dc.identifier.doi","10.1021/jacs.7b08629"],["dc.identifier.pmid","29037034"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/62272"],["dc.language.iso","en"],["dc.notes.status","final"],["dc.relation.eissn","1520-5126"],["dc.relation.issn","0002-7863"],["dc.title","Pairwise H2/D2 Exchange and H2 Substitution at a Bimetallic Dinickel(II) Complex Featuring Two Terminal Hydrides"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]Details DOI PMID PMC2019Journal 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"]]Details DOI