Demeshko, Serhiy V.

[["dc.bibliographiccitation.firstpage","5511"],["dc.bibliographiccitation.issue","40"],["dc.bibliographiccitation.journal","Chemical Communications"],["dc.bibliographiccitation.lastpage","5514"],["dc.bibliographiccitation.volume","53"],["dc.contributor.author","Abbenseth, Josh"],["dc.contributor.author","Diefenbach, Martin"],["dc.contributor.author","Bete, Sarah C."],["dc.contributor.author","Würtele, Christian"],["dc.contributor.author","Volkmann, Christian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Holthausen, Max C."],["dc.contributor.author","Schneider, Sven"],["dc.date.accessioned","2018-08-17T09:33:43Z"],["dc.date.accessioned","2021-10-27T13:12:42Z"],["dc.date.available","2018-08-17T09:33:43Z"],["dc.date.available","2021-10-27T13:12:42Z"],["dc.date.issued","2017"],["dc.description.abstract","Reduction of the pincer complex [OsIIICl2(PNP)] (PNP = N(CHCHPtBu2)2) affords the isolation and full characterization of an osmium(II) complex with square-planar coordination geometry, i.e. [OsIICl(PNP)]. Spectroscopic, structural and magnetic data in combination with multireference computations indicate strong temperature independent paramagnetism, which arises from an energetically well separated ground state that mixes with excited states through spin-orbit coupling."],["dc.identifier.doi","10.1039/C7CC01569K"],["dc.identifier.isi","000401602900006"],["dc.identifier.pmid","28405639"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/15307"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/91714"],["dc.language.iso","en"],["dc.notes.intern","Migrated from goescholar"],["dc.notes.intern","In goescholar not merged with http://resolver.sub.uni-goettingen.de/purl?gs-1/15078 but duplicate"],["dc.relation","info:eu-repo/grantAgreement/EC/H2020/646747/EU//N2FEED"],["dc.relation.eissn","1364-548X"],["dc.relation.issn","1359-7345"],["dc.relation.orgunit","Fakultät für Chemie"],["dc.rights","Goescholar"],["dc.rights.access","openAccess"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.subject","Complex; Square-Planar; Osmium(II)"],["dc.subject.ddc","540"],["dc.title","A Square-Planar Osmium(II) Complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.version","submitted_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","10428"],["dc.bibliographiccitation.issue","37"],["dc.bibliographiccitation.journal","Chemical Communications"],["dc.bibliographiccitation.lastpage","10430"],["dc.bibliographiccitation.volume","47"],["dc.contributor.author","Burger, Boris"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Grosse, Christian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2018-11-07T09:00:57Z"],["dc.date.available","2018-11-07T09:00:57Z"],["dc.date.issued","2011"],["dc.description.abstract","A novel pyrazolate-based diiron(II) complex shows five different binding modes of exogenous carboxylate ligands in a single crystal structure. Temperature dependent X-ray data reveal thermally induced disorder due to carboxylate dynamics that resemble the carboxylate shift, as it is known from various diiron enzyme active sites."],["dc.description.sponsorship","DFG [IRTG 1422]; Evonik Foundation"],["dc.identifier.doi","10.1039/c1cc13756e"],["dc.identifier.isi","000294500600072"],["dc.identifier.pmid","21842055"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/8677"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/24289"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1364-548X"],["dc.relation.issn","1359-7345"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Visualising the carboxylate shift at a bioinspired diiron(II) site in the solid state"],["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","4137"],["dc.bibliographiccitation.issue","43"],["dc.bibliographiccitation.journal","European Journal of Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","4145"],["dc.bibliographiccitation.volume","2020"],["dc.contributor.author","Wong, Joanne W. L."],["dc.contributor.author","Hua, Shao‐An"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Ye, Shengfa"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2021-04-14T08:32:19Z"],["dc.date.available","2021-04-14T08:32:19Z"],["dc.date.issued","2020"],["dc.description.abstract","Using a new bis(tridentate) compartmental pyrazolate‐centered ligand HL, the bis(pyrazolato)‐bridged diiron complex [L2FeII2][OTf]2 (1) and its singly oxidized mixed‐valent congener [L2FeIIFeIII][OTf]3 (2) have been synthesized and structurally characterized. While 1 features two HS‐FeII ions coordinated to two cis‐axial pyridine moieties in a highly distorted octahedral environment, the metal ions in 2 are coordinated by the ligand strand in a trans‐axial configuration. Very different Fe–N bond lengths and distinctly different coordination polyhedra are associated with pronounced valence localization in the case of 2. The electronic structures and magnetic properties of 1 and 2 have been further investigated by Mössbauer spectroscopy and variable temperature magnetic susceptibility measurements. In the case of 1, weak antiferromagnetic coupling is observed between the two HS‐FeII ions (J = –0.6 cm–1), while the HS‐FeII and LS‐FeIII ions in 2 are ferromagnetically coupled (J = +5.2 cm–1) to give an ST = 5/2 ground state with significant zero‐field splitting (DFe(II) = 2.3 cm–1). The findings are rationalized with the help of DFT computations."],["dc.description.abstract","Dinuclear iron complexes of a new pyrazolate‐based ligand with flexible side arms were synthesized in both the FeII2 and mixed‐valent FeIIFeIII forms. Upon oxidation, large structural changes were observed, associated with a high‐spin to low‐spin transition and charge localization. The different magnetic signatures of the two compounds were evidenced by a suite of experimental methods and investigated by DFT calculations. image John Wiley \\u0026 Sons, Ltd."],["dc.description.sponsorship","Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659"],["dc.description.sponsorship","Max‐Planck‐Gesellschaft http://dx.doi.org/10.13039/501100004189"],["dc.identifier.doi","10.1002/ejic.202000697"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/83884"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-399"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area B | B06 Echtzeituntersuchungen der optischen Anregung in oligonuklearen Metallkomplexen mit schaltbaren Spin- und Ladungszuständen"],["dc.relation.eissn","1099-0682"],["dc.relation.issn","1434-1948"],["dc.rights","This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes."],["dc.title","Bis(pyrazolato) Bridged Diiron Complexes: Ferromagnetic Coupling in a Mixed‐Valent HS‐Fe II /LS‐Fe III Dinuclear Complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["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","1402"],["dc.bibliographiccitation.issue","15-16"],["dc.bibliographiccitation.journal","European Journal of Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","1410"],["dc.bibliographiccitation.volume","2020"],["dc.contributor.author","van Alten, Richt S."],["dc.contributor.author","Wätjen, Florian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Miller, Alexander J. M."],["dc.contributor.author","Würtele, Christian"],["dc.contributor.author","Siewert, Inke"],["dc.contributor.author","Schneider, Sven"],["dc.date.accessioned","2020-12-10T14:06:28Z"],["dc.date.available","2020-12-10T14:06:28Z"],["dc.date.issued","2020"],["dc.description.abstract","The splitting of N2 into well‐defined terminal nitride complexes is a key reaction for nitrogen fixation at ambient conditions. In continuation of our previous work on rhenium pincer mediated N2 splitting, nitrogen activation and cleavage upon (electro)chemical reduction of [ReCl2(L2)] {L2 = N(CHCHPtBu2)2–} is reported. The electrochemical characterization of [ReCl2(L2)] and comparison with our previously reported platform [ReCl2(L1)] {L1 = N(CH2CH2PtBu2)2–} provides mechanistic insight to rationalize the dependence of nitride yield on the reductant. Furthermore, the reactivity of N2 derived nitride complex [Re(N)Cl(L2)] with electrophiles is presented."],["dc.description.abstract","N2 splitting into terminal nitrides by chemical and electrochemical reduction of [ReCl2{N(CHCHPtBu2)2}] is presented. Comparison of electrochemical data with that of the previously reported, related pincer complex [ReCl2{N(CH2CH2PtBu2)2}] allowed for identifying key parameters that control the efficiency of the reaction sequence, which defines reductive N2 splitting. image John Wiley \\u0026 Sons, Ltd."],["dc.description.sponsorship","European Research Council http://dx.doi.org/10.13039/501100000781"],["dc.description.sponsorship","National Science Foundation"],["dc.identifier.doi","10.1002/ejic.201901278"],["dc.identifier.issn","1434-1948"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/69904"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.rights","This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited."],["dc.title","(Electro-)chemical Splitting of Dinitrogen with a Rhenium Pincer Complex"],["dc.title.alternative","(Electro-)chemical Splitting of Dinitrogen with a Rhenium Pincer Complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","5117"],["dc.bibliographiccitation.issue","14"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","5124"],["dc.bibliographiccitation.volume","139"],["dc.contributor.author","Bagh, Bidraha"],["dc.contributor.author","Broere, Daniel L. J."],["dc.contributor.author","Sinha, Vivek"],["dc.contributor.author","Kuijpers, Petrus F."],["dc.contributor.author","van Leest, Nicolaas P."],["dc.contributor.author","de Bruin, Bas"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Siegler, Maxime A."],["dc.contributor.author","van der Vlugt, Jan Ivar"],["dc.date.accessioned","2018-11-07T10:25:00Z"],["dc.date.available","2018-11-07T10:25:00Z"],["dc.date.issued","2017"],["dc.description.abstract","Coordination of FeCl3 to the redox-active pyridine-aminophenol ligand NNOH2 in the presence of base and under aerobic conditions generates FeCl2(NNOISQ) (1), featuring high-spin Fe-III and an NNOISQ radical ligand. The complex has an overall S = 2 spin state, as deduced from experimental and computational data. The ligand-centered radical couples antiferromagnetically with the Fe center. Readily available, well-defined, and air-stable 1 catalyzes the challenging intramolecular direct C(sp(3))-H amination of unactivated organic azides to generate a range of saturated N-heterocycles with the highest turnover number (TON) (1 mol% of 1, 12 h, TON = 62; 0.1 mol% of 1, 7 days, TON = 620) reported to date. The catalyst is easily recycled without noticeable loss of catalytic activity. A detailed kinetic study for C(sp(3))-H amination of 1-azido-4-phenylbutane (S-1) revealed zero order in the azide substrate and first order in both the catalyst and Boc(2)O. A cationic iron complex, generated from the neutral precatalyst upon reaction with Boc(2)O, is proposed as the catalytically active species."],["dc.identifier.doi","10.1021/jacs.7b00270"],["dc.identifier.isi","000399353800026"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/14461"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/42766"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","PUB_WoS_Import"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0002-7863"],["dc.rights","CC BY-NC-ND 3.0"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc-nd/3.0"],["dc.title","Catalytic Synthesis of N-Heterocycles via Direct C(sp(3))-H Amination Using an Air-Stable Iron(III) Species with a Redox-Active Ligand"],["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"]]

[["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"]]

[["dc.bibliographiccitation.firstpage","1891"],["dc.bibliographiccitation.issue","4"],["dc.bibliographiccitation.journal","Angewandte Chemie. International Edition"],["dc.bibliographiccitation.lastpage","1896"],["dc.bibliographiccitation.volume","60"],["dc.contributor.author","Duan, Peng-Cheng"],["dc.contributor.author","Schulz, Roland Alexander"],["dc.contributor.author","Römer, Anton"],["dc.contributor.author","Van Kuiken, Benjamin E."],["dc.contributor.author","Dechert, Sebastian"],["dc.contributor.author","Demeshko, Serhiy"],["dc.contributor.author","Cutsail, George E."],["dc.contributor.author","DeBeer, Serena"],["dc.contributor.author","Mata, Ricardo"],["dc.contributor.author","Meyer, Franc"],["dc.date.accessioned","2020-11-05T14:37:43Z"],["dc.date.available","2020-11-05T14:37:43Z"],["dc.date.issued","2020"],["dc.description.abstract","Abstract The dinickel(II) dihydride complex (1K) of a pyrazolate‐based compartmental ligand with β‐diketiminato (nacnac) chelate arms (L−), providing two pincer‐type {N3} binding pockets, has been reported to readily eliminate H2 and to serve as a masked dinickel(I) species. Discrete dinickel(I) complexes (2Na, 2K) of L− are now synthesized via a direct reduction route. They feature two adjacent T‐shaped metalloradicals that are antiferromagnetically coupled, giving an S=0 ground state. The two singly occupied local dx2-y2 type magnetic orbitals are oriented into the bimetallic cleft, enabling metal–metal cooperative 2 e− substrate reductions as shown by the rapid reaction with H2 or O2. X‐ray crystallography reveals distinctly different positions of the K+ in 1K and 2K, suggesting a stabilizing interaction of K+ with the dihydride unit in 1K. H2 release from 1K is triggered by peripheral γ‐C protonation at the nacnac subunits, which DFT calculations show lowers the barrier for reductive H2 elimination from the bimetallic cleft."],["dc.description.abstract","Highly reactive dinickel(I) complexes with an open cleft between two “T”‐shaped metalloradicals are accessible via H2 release from a dinickel(II) dihydride complex based on a pyrazolate/β‐diketiminato hybrid ligand. The barrier to intramolecular H2 elimination is drastically lowered by protonation at the ligand periphery. image"],["dc.description.sponsorship","Deutsche Forschungsgemeinschaft http://dx.doi.org/10.13039/501100001659"],["dc.description.sponsorship","China Scholarship Council http://dx.doi.org/10.13039/501100004543"],["dc.description.sponsorship","Max-Planck-Gesellschaft http://dx.doi.org/10.13039/501100004189"],["dc.identifier.doi","10.1002/anie.202011494"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/68171"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-352"],["dc.relation.eissn","1521-3773"],["dc.relation.issn","1433-7851"],["dc.rights","This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes."],["dc.title","Ligand Protonation Triggers H2 Release from a Dinickel Dihydride Complex to Give a Doubly “T”‐Shaped Dinickel(I) Metallodiradical"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]