TY - JOUR AU - Köring, Laura AU - Stepen, Arne AU - Birenheide, Bernhard AU - Barth, Simon AU - Leskov, Maxim AU - Schoch, Roland AU - Krämer, Felix AU - Breher, Frank AU - Paradies, Jan ID - 35694 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Boron‐Centered Lewis Superacid through Redox‐Active Ligands: Application in C–F and S–F Bond Activation ER - TY - JOUR AU - Liang, Qian AU - Ma, Xuekai AU - Long, Teng AU - Yao, Jiannian AU - Liao, Qing AU - Fu, Hongbing ID - 35077 IS - 9 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Circularly Polarized Lasing from a Microcavity Filled with Achiral Single‐Crystalline Microribbons VL - 62 ER - TY - JOUR AU - Köring, Laura AU - Stepen, Arne AU - Birenheide, Bernhard AU - Barth, Simon AU - Leskov, Maxim AU - Schoch, Roland AU - Krämer, Felix AU - Breher, Frank AU - Paradies, Jan ID - 42878 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Boron‐Centered Lewis Superacid through Redox‐Active Ligands: Application in C−F and S−F Bond Activation ER - TY - JOUR AB - Faradaic reactions including charge transfer are often accompanied with diffusion limitation inside the bulk. Conductive two-dimensional frameworks (2D MOFs) with a fast ion transport can combine both - charge transfer and fast diffusion inside their porous structure. To study remaining diffusion limitations caused by particle morphology, different synthesis routes of Cu-2,3,6,7,10,11-hexahydroxytriphenylene (Cu3(HHTP)2), a copper-based 2D MOF, are used to obtain flake- and rod-like MOF particles. Both morphologies are systematically characterized and evaluated for redox-active Li+ ion storage. The redox mechanism is investigated by means of X-ray absorption spectroscopy, FTIR spectroscopy and in situ XRD. Both types are compared regarding kinetic properties for Li+ ion storage via cyclic voltammetry and impedance spectroscopy. A significant influence of particle morphology for 2D MOFs on kinetic aspects of electrochemical Li+ ion storage can be observed. This study opens the path for optimization of redox active porous structures to overcome diffusion limitations of Faradaic processes. AU - Wrogemann, Jens Matthies AU - Lüther, Marco Joes AU - Bärmann, Peer AU - Lounasvuori, Mailis AU - Javed, Ali AU - Tiemann, Michael AU - Golnak, Ronny AU - Xiao, Jie AU - Petit, Tristan AU - Placke, Tobias AU - Winter, Martin ID - 44116 IS - 26 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Overcoming Diffusion Limitation of Faradaic Processes: Property‐Performance Relationships of 2D Conductive Metal‐Organic Framework Cu3(HHTP)2 for Reversible Lithium‐Ion Storage VL - 62 ER - TY - JOUR AU - Sieland, Benedikt AU - Stahn, Marcel AU - Schoch, Roland AU - Daniliuc, Constantin AU - Spicher, Sebastian AU - Grimme, Stefan AU - Hansen, Andreas AU - Paradies, Jan ID - 46277 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Dispersion Energy‐Stabilized Boron and Phosphorus Lewis Pairs ER - TY - JOUR AU - Wicker, Garrit AU - Zhou, Rundong AU - Schoch, Roland AU - Paradies, Jan ID - 35689 IS - 31 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Sigmatropic [1,5] Carbon Shift of Transient C3 Ammonium Enolates VL - 61 ER - TY - JOUR AU - Wicker, Garrit AU - Zhou, Rundong AU - Schoch, Roland AU - Paradies, Jan ID - 35691 IS - 31 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Cover Picture: Sigmatropic [1,5] Carbon Shift of Transient C3 Ammonium Enolates (Angew. Chem. Int. Ed. 31/2022) VL - 61 ER - TY - JOUR AU - Lepre, Enrico AU - Rat, Sylvain AU - Cavedon, Cristian AU - Seeberger, Peter H. AU - Pieber, Bartholomäus AU - Antonietti, Markus AU - Lopez Salas, Nieves ID - 40555 IS - 2 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Catalytic Properties of High Nitrogen Content Carbonaceous Materials VL - 62 ER - TY - JOUR AU - Tian, Zhihong AU - Zhang, Qingran AU - Thomsen, Lars AU - Gao, Nana AU - Pan, Jian AU - Daiyan, Rahman AU - Yun, Jimmy AU - Brandt, Jessica AU - Lopez Salas, Nieves AU - Lai, Feili AU - Li, Qiuye AU - Liu, Tianxi AU - Amal, Rose AU - Lu, Xunyu AU - Antonietti, Markus ID - 40560 IS - 37 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Constructing Interfacial Boron‐Nitrogen Moieties in Turbostratic Carbon for Electrochemical Hydrogen Peroxide Production VL - 61 ER - TY - JOUR AU - Gurinov, Andrei AU - Sieland, Benedikt AU - Kuzhelev, Andrey AU - Elgabarty, Hossam AU - Kühne, Thomas AU - Prisner, Thomas AU - Paradies, Jan AU - Baldus, Marc AU - Ivanov, Konstantin L. AU - Pylaeva, Svetlana ID - 33653 IS - 28 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Mixed‐Valence Compounds as Polarizing Agents for Overhauser Dynamic Nuclear Polarization in Solids VL - 60 ER - TY - JOUR AU - Gurinov, Andrei AU - Benedikt, Sieland AU - Kuzhelev, Andrey AU - Elgabarty, Hossam AU - Kühne, Thomas D AU - Prisner, Thomas AU - Paradies, Jan AU - Baldus, Marc AU - Ivanov, Konstantin L AU - Pylaeva, Svetlana ID - 22231 JF - Angewandte Chemie International Edition SN - 1433-7851 TI - Mixed‐valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids ER - TY - JOUR AB - Metal-catalyzed C−H activations are environmentally and economically attractive synthetic strategies for the construction of functional molecules as they obviate the need for pre-functionalized substrates and minimize waste generation. Great challenges reside in the control of selectivities, the utilization of unbiased hydrocarbons, and the operation of atom-economical dehydrocoupling mechanisms. An especially mild borylation of benzylic CH bonds was developed with the ligand-free pre-catalyst Co[N(SiMe3)2]2 and the bench-stable and inexpensive borylation reagent B2pin2 that produces H2 as the only by-product. A full set of kinetic, spectroscopic, and preparative mechanistic studies are indicative of a tandem catalysis mechanism of CH-borylation and dehydrocoupling via molecular CoI catalysts. AU - Ghosh, Pradip AU - Schoch, Roland AU - Bauer, Matthias AU - Jacobi von Wangelin, Axel ID - 41000 IS - 1 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Selective Benzylic CH‐Borylations by Tandem Cobalt Catalysis VL - 61 ER - TY - JOUR AB - We present the η3-coordination of the 2-phosphaethynthiolate anion in the complex (PN)2La(SCP) (2) [PN=N-(2-(diisopropylphosphanyl)-4-methylphenyl)-2,4,6-trimethylanilide)]. Structural comparison with dinuclear thiocyanate-bridged (PN)2La(μ-1,3-SCN)2La(PN)2 (3) and azide-bridged (PN)2La(μ-1,3-N3)2La(PN)2 (4) complexes indicates that the [SCP]− coordination mode is mainly governed by electronic, rather than steric factors. Quantum mechanical investigations reveal large contributions of the antibonding π*-orbital of the [SCP]− ligand to the LUMO of complex 2, rendering it the ideal precursor for the first functionalization of the [SCP]− anion. Complex 2 was therefore reacted with CAACs which induced a selective rearrangement of the [SCP]− ligand to form the first CAAC stabilized group 15–group 16 fulminate-type complexes (PN)2La{SPC(RCAAC)} (5 a,b, R=Ad, Me). A detailed reaction mechanism for the SCP-to-SPC isomerization is proposed based on DFT calculations. AU - Watt, Fabian A. AU - Burkhardt, Lukas AU - Schoch, Roland AU - Mitzinger, Stefan AU - Bauer, Matthias AU - Weigend, Florian AU - Goicoechea, Jose M. AU - Tambornino, Frank AU - Hohloch, Stephan ID - 41010 IS - 17 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - η 3 ‐Coordination and Functionalization of the 2‐Phosphaethynthiolate Anion at Lanthanum(III)** VL - 60 ER - TY - JOUR AU - Su, Ran AU - Wang, Zhipeng AU - Zhu, Lina AU - Pan, Ying AU - Zhang, Dawei AU - Wen, Hui AU - Luo, Zheng‐Dong AU - Li, Linglong AU - Li, Fa‐tang AU - Wu, Ming AU - He, Liqiang AU - Sharma, Pankaj AU - Seidel, Jan ID - 46000 IS - 29 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Strain‐Engineered Nano‐Ferroelectrics for High‐Efficiency Piezocatalytic Overall Water Splitting VL - 60 ER - TY - JOUR AB - Exceptionally electron-rich, nearly trigonal-planar tricyanidometalate anions [Fe(CN)3]7− and [Ru(CN)3]7− were stabilized in LiSr3[Fe(CN)3] and AE3.5[M(CN)3] (AE=Sr, Ba; M=Fe, Ru). They are the first examples of group 8 elements with the oxidation state of −IV. Microcrystalline powders were obtained by a solid-state route, single crystals from alkali metal flux. While LiSr3[Fe(CN)3] crystallizes in P63/m, the polar space group P63 with three-fold cell volume for AE3.5[M(CN)3] is confirmed by second harmonic generation. X-ray diffraction, IR and Raman spectroscopy reveal longer C−N distances (124–128 pm) and much lower stretching frequencies (1484–1634 cm−1) than in classical cyanidometalates. Weak C−N bonds in combination with strong M−C π-bonding is a scheme also known for carbonylmetalates. Instead of the formal notation [Fe−IV(CN−)3]7−, quantum chemical calculations reveal non-innocent intermediate-valent CN1.67− ligands and a closed-shell d10 configuration for Fe, that is, Fe2−. AU - Jach, Franziska AU - Wagner, Frank R. AU - Amber, Zeeshan H. AU - Rüsing, Michael AU - Hunger, Jens AU - Prots, Yurii AU - Kaiser, Martin AU - Bobnar, Matej AU - Jesche, Anton AU - Eng, Lukas M. AU - Ruck, Michael AU - Höhn, Peter ID - 47965 IS - 29 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Tricyanidoferrates(−IV) and Ruthenates(−IV) with Non‐Innocent Cyanido Ligands VL - 60 ER - TY - JOUR AU - Steinrück, Hans-Georg AU - Cao, Chuntian AU - Lukatskaya, Maria R. AU - Takacs, Christopher J. AU - Wan, Gang AU - Mackanic, David G. AU - Tsao, Yuchi AU - Zhao, Jingbo AU - Helms, Brett A. AU - Xu, Kang AU - Borodin, Oleg AU - Wishart, James F. AU - Toney, Michael F. ID - 23606 JF - Angewandte Chemie International Edition SN - 1433-7851 TI - Interfacial Speciation Determines Interfacial Chemistry: X‐ray‐Induced Lithium Fluoride Formation from Water‐in‐salt Electrolytes on Solid Surfaces VL - 59 ER - TY - JOUR AU - Kielar, Charlotte AU - Zhu, Siqi AU - Grundmeier, Guido AU - Keller, Adrian ID - 22647 JF - Angewandte Chemie International Edition SN - 1433-7851 TI - Quantitative Assessment of Tip Effects in Single‐Molecule High‐Speed Atomic Force Microscopy Using DNA Origami Substrates VL - 59 ER - TY - JOUR AU - Keller, Adrian AU - Linko, Veikko ID - 22650 JF - Angewandte Chemie International Edition SN - 1433-7851 TI - Challenges and Perspectives of DNA Nanostructures in Biomedicine VL - 59 ER - TY - JOUR AU - Longwitz, Lars AU - Werner, Thomas ID - 37954 IS - 7 JF - Angewandte Chemie International Edition KW - General Chemistry KW - Catalysis SN - 1433-7851 TI - Reduction of Activated Alkenes by P III /P V Redox Cycling Catalysis VL - 59 ER - TY - JOUR AU - Stepen, Arne J. AU - Bursch, Markus AU - Grimme, Stefan AU - Stephan, Douglas W. AU - Paradies, Jan ID - 22241 JF - Angewandte Chemie International Edition SN - 1433-7851 TI - Electrophilic Phosphonium Cation‐Mediated Phosphane Oxide Reduction Using Oxalyl Chloride and Hydrogen ER -