Items 1-20 of 614

    • Journal Article

      A platinum(ii) metallonitrene with a triplet ground state 

      Sun, Jian; Abbenseth, Josh; Verplancke, Hendrik; Diefenbach, Martin; de Bruin, Bas; Hunger, David; Würtele, Christian; van Slageren, Joris; Holthausen, Max C.; Schneider, Sven
      Nature Chemistry 2020; 12(11) p.1054-1059
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    • Journal Article

      Examination of Protonation-Induced Dinitrogen Splitting by in Situ EXAFS Spectroscopy 

      Abbenseth, Josh; Oudsen, Jean-Pierre H.; Venderbosch, Bas; Demeshko, Serhiy; Finger, Markus; Herwig, Christian; Würtele, Christian; Holthausen, Max C.; Limberg, Christian; Tromp, Moniek; et al.
      Schneider, Sven
      Inorganic Chemistry 2020; 59(19) p.14367-14375
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    • Journal Article

      Nitrogen Fixation via Splitting into Nitrido Complexes 

      Forrest, Sebastian J. K.; Schluschaß, Bastian; Yuzik-Klimova, Ekaterina Y.; Schneider, Sven
      Chemical Reviews 2021; 121(11) p.6522-6587
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    • Journal Article

      Stabilizing P≡P: P22–, P2⋅–, and P20 as bridging ligands 

      Sun, Jian; Verplancke, Hendrik; Schweizer, Julia I.; Diefenbach, Martin; Würtele, Christian; Otte, Matthias; Tkach, Igor; Herwig, Christian; Limberg, Christian; Demeshko, Serhiy; et al.
      Holthausen, Max C.Schneider, Sven
      Chem 2021; 7(7) p.1952-1962
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    • Journal Article

      Remote near infrared identification of pathogens with multiplexed nanosensors 

      Nißler, Robert; Bader, Oliver; Dohmen, Maria; Walter, Sebastian G.; Noll, Christine; Selvaggio, Gabriele; Groß, Uwe; Kruss, Sebastian
      Nature Communications 2020; 11(1)
      Infectious diseases are worldwide a major cause of morbidity and mortality. Fast and specific detection of pathogens such as bacteria is needed to combat these diseases. Optimal methods would be non-invasive and without extensive sample-taking/processing. Here, we developed a set of near infrared (NIR) fluorescent nanosensors and used them for remote fingerprinting of clinically important bacteria. The nanosensors are based on single-walled carbon nanotubes (SWCNTs) that fluoresce in the NIR optical tissue transparency window, which offers ultra-low background and high tissue penetration. They are chemically tailored to detect released metabolites as well as specific virulence factors (lipopolysaccharides, siderophores, DNases, proteases) and integrated into functional hydrogel arrays with 9 different sensors. These hydrogels are exposed to clinical isolates of 6 important bacteria (Staphylococcus aureus, Escherichia coli,…) and remote (≥25 cm) NIR imaging allows to identify and distinguish bacteria. Sensors are also spectrally encoded (900 nm, 1000 nm, 1250 nm) to differentiate the two major pathogens P. aeruginosa as well as S. aureus and penetrate tissue (>5 mm). This type of multiplexing with NIR fluorescent nanosensors enables remote detection and differentiation of important pathogens and the potential for smart surfaces.
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    • Journal Article

      A fourth-generation high-dimensional neural network potential with accurate electrostatics including non-local charge transfer 

      Ko, Tsz Wai; Finkler, Jonas A.; Goedecker, Stefan; Behler, Jörg
      Nature Communications 2021; 12(1)
      Machine learning potentials have become an important tool for atomistic simulations in many fields, from chemistry via molecular biology to materials science. Most of the established methods, however, rely on local properties and are thus unable to take global changes in the electronic structure into account, which result from long-range charge transfer or different charge states. In this work we overcome this limitation by introducing a fourth-generation high-dimensional neural network potential that combines a charge equilibration scheme employing environment-dependent atomic electronegativities with accurate atomic energies. The method, which is able to correctly describe global charge distributions in arbitrary systems, yields much improved energies and substantially extends the applicability of modern machine learning potentials. This is demonstrated for a series of systems representing typical scenarios in chemistry and materials science that are incorrectly described by current methods, while the fourth-generation neural network potential is in excellent agreement with electronic structure calculations.
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    • Journal Article

      Polymorphism of bis(1,3-benzothiazol-2-yl) trithiocarbonate 

      Kafuta, Kevin; Golz, Christopher; Alcarazo, Manuel
      Acta Crystallographica Section E Crystallographic Communications 2020; 76(7) p.1126-1130
      The polymorphism of the title compound, C15H8N2S5, is reported, in which the (syn,syn) and (syn,anti) conformers simultaneously crystallized from a chloroform solution. The complete molecule of the (syn,syn) form is generated by a crystallographic twofold axis. The geometries of both conformers are compared in detail, revealing no significant differences in bond lengths, despite different bond angles because of the conformational changes. Analysis of the intermolecular interactions, aided by Hirshfeld surfaces, shows distinctive SS and SN contacts only for the (syn,anti) conformer. Aromatic –-stacking interactions are found for both conformers, which occur for the (syn,anti) conformer between pairs of molecules, but are continuous stacks in the (syn,syn) conformer. Non merohedral twinning was found for the crystal of the (syn,anti) conformer used for data collection.
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    • Journal Article

      Mesoporous-silica-coated palladium-nanocubes as recyclable nanocatalyst in C–C-coupling reaction – a green approach 

      Rohleder, Darius; Vana, Philipp
      RSC Advances 2020; 10(44) p.26504-26507
      We report the straightforward design of a recyclable palladium-core–silica-shell nanocatalyst showing an excellent balance between sufficient stability and permeability. The overall process – design, catalysis and purification – is characterized by its sustainability and simplicity accompanied by a great recycling potential and ultra high yields in C–C-coupling reactions.
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    • Journal Article

      Exfoliated near infrared fluorescent silicate nanosheets for (bio)photonics 

      Selvaggio, Gabriele; Chizhik, Alexey; Nißler, Robert; Kuhlemann, llyas; Meyer, Daniel; Vuong, Loan; Preiß, Helen; Herrmann, Niklas; Mann, Florian A.; Lv, Zhiyi; et al.
      Oswald, Tabea A.Spreinat, AlexanderErpenbeck, LuiseGroßhans, JörgKarius, VolkerJanshoff, AndreasPablo Giraldo, JuanKruss, Sebastian
      Nature Communications 2020; 11(1) p.1-11: Art. 1495
      Imaging of complex (biological) samples in the near-infrared (NIR) is beneficial due toreduced light scattering, absorption, phototoxicity, and autofluorescence. However, there arefew NIRfluorescent materials known and suitable for biomedical applications. Here weexfoliate the layered pigment $CaCuSi_4O_{10}$ (Egyptian Blue, EB) via ball milling and facile tipsonication into NIRfluorescent nanosheets (EB-NS). The size of EB-NS can be tailored todiameters <20 nm and heights down to 1 nm. EB-NSfluoresce at 910 nm and thefluorescenceintensity correlates with the number of $Cu^{2+}$ ions. Furthermore, EB-NS display no bleachingand high brightness compared with other NIRfluorophores. The versatility of EB-NS isdemonstrated by in-vivo single-particle tracking and microrheology measurements inDro-sophila melanogasterembryos. EB-NS can be uptaken by plants and remotely detected in alow-cost stand-off detection setup. In summary, EB-NS have the potential for a wide range ofbioimaging applications.
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    • Journal Article

      Electrochemical Access to Aza-Polycyclic Aromatic Hydrocarbons: Rhoda-Electrocatalyzed Domino Alkyne Annulations 

      Kong, Wei-Jun; Shen, Zhigao; Finger, Lars H.; Ackermann, Lutz
      Angewandte Chemie International Edition(59) p.1-7
      Nitrogen-doped polycyclic aromatic hydrocarbons (aza-PAHs) have found broad applications in material sciences. Herein, a modular electrochemical synthesis of aza-PAHs was developed via a rhodium-catalyzed cascade C-H activation and alkyne annulation. A multifunctional O-methylamidoxime enabled the high chemo- and regioselectivity. The isolation of two key rhodacyclic intermediates made it possible to delineate the exact order of three C-H activation steps. In addition, the metalla-electrocatalyzed multiple C-H transformation is characterized by unique functional group tolerance, including highly reactive iodo and azido groups.
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    • Journal Article

      An Unprecedented Fully H - Substituted Phosphate Hydride Sr5(PO4)3H Expanding the Apatite Family 

      Mutschke, Alexander; Wylezich, Thomas; Ritter, Clemens; Karttunen, Antti J.; Kunkel, Nathalie
      European Journal of Inorganic Chemistry 2019; 2019(48) p.5073-5076
      The apatite family is a mineral class that also contains the biologically very important hydroxyapatite. Here, we are reporting on the synthesis and characterization of a fully hydride‐substituted strontium apatite, which could be obtained via mechanochemical synthesis and subsequent annealing treatment. The full substitution by hydride anions is proven by various methods, such as neutron powder diffraction of a deuterated sample Sr5(PO4)3D, as well 1H MAS solid state NMR combined with quantum chemical calculations, vibrational spectroscopy and elemental analysis. The present work expands the apatite family from the known halide and hydroxide apatites to the fully hydride‐anion‐substituted variant and is expected to open up a new field of materials containing coexistent phosphate and hydride anions.
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    • Journal Article

      Sequential Double Dearomatization of the Pyrazolate-Based “Two-in-One” Pincer Ligand in a Dinuclear Rhodium(I) Complex 

      Gers-Barlag, Alexander; Goursot, Pierre; Li, Ming; Dechert, Sebastian; Meyer, Franc
      European Journal of Inorganic Chemistry 2019; 2019(28) p.3329-3334
      A binucleating pyrazolate‐based ligand providing two tridentate PNN compartments is shown to form a dinuclear rhodium(I) complex [L{Rh(CO)}2](PF6) (1) that can be deprotonated at both side arm methylene groups between pyridine and phosphino donors to give K[L**{Rh(CO)}2] (3). Sequential twofold deprotonation has been monitored by NMR and UV/Vis spectroscopy and proceeds via the neutral intermediate L*{Rh(CO)}2 (2). X‐ray crystallographic characterization of 1 and the K[2,2,2]+ salt 3′ ([2,2,2] is a cryptand) evidences pyridine dearomatization upon deprotonation, and all spectroscopic and structural signatures are in good agreement with those of related mononuclear rhodium complexes based on a common PNN pincer ligand, which corroborates that pyrazolate‐bridged L– is best described as a scaffold with two pincer‐type subunits.
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    • Journal Article

      Oxidative Coupling of Terminal Rhenium Pnictide Complexes 

      Abbenseth, Josh; Diefenbach, Martin; Hinz, Alexander; Alig, Lukas; Würtele, Christian; Goicoechea, Jose M.; Holthausen, Max C.; Schneider, Sven
      Angewandte Chemie International Edition 2019; 58(32) p.10966-10970
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    • Journal Article

      A Terminal Iridium Oxo Complex with a Triplet Ground State 

      Delony, Daniel; Kinauer, Markus; Diefenbach, Martin; Demeshko, Serhiy; Würtele, Christian; Holthausen, Max C.; Schneider, Sven
      Angewandte Chemie International Edition 2019; 58(32) p.10971-10974
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    • Journal Article

      First-Row Transition Metal (De)Hydrogenation Catalysis Based On Functional Pincer Ligands 

      Alig, Lukas; Fritz, Maximilian; Schneider, Sven
      Chemical Reviews 2018; 119(4) p.2681-2751
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    • Journal Article

      Metal-Ligand Cooperative Synthesis of Benzonitrile by Electrochemical Reduction and Photolytic Splitting of Dinitrogen 

      Schendzielorz, Florian; Finger, Markus; Abbenseth, Josh; Würtele, Christian; Krewald, Vera; Schneider, Sven
      Angewandte Chemie International Edition 2018; 58(3) p.830-834
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    • Journal Article

      Iron‐Electrocatalyzed C−H Arylations: Mechanistic Insights into Oxidation‐Induced Reductive Elimination for Ferraelectrocatalysis 

      Zhu, Cuiju; Stangier, Maximilian; Oliveira, João C. A.; Massignan, Leonardo; Ackermann, Lutz
      Chemistry – A European Journal 2019; 25(71) p.16382-16389
      Despite major advances, organometallic C-H transformations are dominated by precious 5d and 4d transition metals, such as iridium, palladium and rhodium. In contrast, the unique potential of less toxic Earth-abundant 3d metals has been underexplored. While iron is the most naturally abundant transition metal, its use in oxidative, organometallic C-H activation has faced major limitations due to the need for superstoichiometric amounts of corrosive, cost-intensive DCIB as the sacrificial oxidant. To fully address these restrictions, we describe herein the unprecedented merger of electrosynthesis with iron-catalyzed C-H activation through oxidation-induced reductive elimination. Thus, ferra- and manganaelectro-catalyzed C-H arylations were accomplished at mild reaction temperatures with ample scope by the action of sustainable iron catalysts, employing electricity as a benign oxidant.
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    • Journal Article

      Hydrosilane Synthesis by Catalytic Hydrogenolysis of Chlorosilanes and Silyl Triflates 

      Glüer, Arne; Schweizer, Julia I.; Karaca, Uhut S.; Würtele, Christian; Diefenbach, Martin; Holthausen, Max C.; Schneider, Sven
      Inorganic Chemistry 2018; 57(21) p.13822-13828
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    • Journal Article

      Iron catalyzed hydrogenation and electrochemical reduction of CO 2 : The role of functional ligands 

      Glüer, Arne; Schneider, Sven
      Journal of Organometallic Chemistry 2018; 861 p.159-173
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    • Journal Article

      Synthesis of Benzonitrile from Dinitrogen 

      Klopsch, Isabel; Schendzielorz, Florian; Volkmann, Christian; Würtele, Christian; Schneider, Sven
      Zeitschrift für anorganische und allgemeine Chemie 2018; 644(17) p.916-919
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