Würtele, Christian

[["dc.bibliographiccitation.firstpage","7922"],["dc.bibliographiccitation.issue","25"],["dc.bibliographiccitation.journal","Journal of the American Chemical Society"],["dc.bibliographiccitation.lastpage","7935"],["dc.bibliographiccitation.volume","140"],["dc.contributor.author","Lindley, Brian M."],["dc.contributor.author","van Alten, Richt S."],["dc.contributor.author","Finger, Markus"],["dc.contributor.author","Schendzielorz, Florian S."],["dc.contributor.author","Würtele, Christian"],["dc.contributor.author","Miller, Alexander J. M."],["dc.contributor.author","Siewert, Inke"],["dc.contributor.author","Schneider, Sven"],["dc.date.accessioned","2019-10-28T10:12:34Z"],["dc.date.available","2019-10-28T10:12:34Z"],["dc.date.issued","2018"],["dc.description.abstract","A comprehensive mechanistic study of N2 activation and splitting into terminal nitride ligands upon reduction of the rhenium dichloride complex [ReCl2(PNP)] is presented (PNP- = N(CH2CH2P tBu2)2-). Low-temperature studies using chemical reductants enabled full characterization of the N2-bridged intermediate [{(PNP)ClRe}2(N2)] and kinetic analysis of the N-N bond scission process. Controlled potential electrolysis at room temperature also resulted in formation of the nitride product [Re(N)Cl(PNP)]. This first example of molecular electrochemical N2 splitting into nitride complexes enabled the use of cyclic voltammetry (CV) methods to establish the mechanism of reductive N2 activation to form the N2-bridged intermediate. CV data was acquired under Ar and N2, and with varying chloride concentration, rhenium concentration, and N2 pressure. A series of kinetic models was vetted against the CV data using digital simulations, leading to the assignment of an ECCEC mechanism (where \"E\" is an electrochemical step and \"C\" is a chemical step) for N2 activation that proceeds via initial reduction to ReII, N2 binding, chloride dissociation, and further reduction to ReI before formation of the N2-bridged, dinuclear intermediate by comproportionation with the ReIII precursor. Experimental kinetic data for all individual steps could be obtained. The mechanism is supported by density functional theory computations, which provide further insight into the electronic structure requirements for N2 splitting in the tetragonal frameworks enforced by rigid pincer ligands."],["dc.identifier.doi","10.1021/jacs.8b03755"],["dc.identifier.pmid","29856611"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/15622"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/62532"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.relation.eissn","1520-5126"],["dc.relation.issn","0002-7863"],["dc.relation.issn","1520-5126"],["dc.relation.orgunit","Institut für Röntgenphysik"],["dc.relation.workinggroup","RG Salditt (Structure of Biomolecular Assemblies and X-Ray Physics)"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.subject.gro","cellular biophysics"],["dc.title","Mechanism of Chemical and Electrochemical N2 Splitting by a Rhenium Pincer Complex"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["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","1348"],["dc.bibliographiccitation.issue","15-16"],["dc.bibliographiccitation.journal","European Journal of Inorganic Chemistry"],["dc.bibliographiccitation.lastpage","1348"],["dc.bibliographiccitation.volume","2020"],["dc.contributor.author","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","2021-12-08T12:30:30Z"],["dc.date.available","2021-12-08T12:30:30Z"],["dc.date.issued","2020"],["dc.identifier.doi","10.1002/ejic.202000342"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/96457"],["dc.language.iso","en"],["dc.notes.intern","DOI-Import GROB-476"],["dc.relation.eissn","1099-0682"],["dc.relation.issn","1434-1948"],["dc.title","Cover Feature: (Electro‐)chemical Splitting of Dinitrogen with a Rhenium Pincer Complex (Eur. J. Inorg. Chem. 15‐16/2020)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]