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 - Within this article, it is shown that an electrochemical defluorination and additional fluorination of Ruddlesden–Popper-type La2NiO3F2 is possible within all-solid-state fluoride-ion batteries. Structural changes within the reduced and oxidized phases have been examined by X-ray diffraction studies at different states of charging and discharging. The synthesis of the oxidized phase La2NiO3F2+x proved to be successful by structural analysis using both X-ray powder diffraction and automated electron diffraction tomography techniques. The structural reversibility on re-fluorinating and re-defluorinating is also demonstrated. Moreover, the influence of different sequences of consecutive reduction and oxidation steps on the formed phases has been investigated. The observed structural changes have been compared to changes in phases obtained via other topochemical modification approaches such as hydride-based reduction and oxidative fluorination using F2 gas, highlighting the potential of such electrochemical reactions as alternative synthesis routes. Furthermore, the electrochemical routes represent safe and controllable synthesis approaches for novel phases, which cannot be synthesized via other topochemical methods. Additionally, side reactions, occurring alongside the desired electrochemical reactions, have been addressed and the cycling performance has been studied.
AU - Wissel, Kerstin
AU - Schoch, Roland
AU - Vogel, Tobias
AU - Donzelli, Manuel
AU - Matveeva, Galina
AU - Kolb, Ute
AU - Bauer, Matthias
AU - Slater, Peter R.
AU - Clemens, Oliver
ID - 41013
IS - 2
JF - Chemistry of Materials
KW - Materials Chemistry
KW - General Chemical Engineering
KW - General Chemistry
SN - 0897-4756
TI - Electrochemical Reduction and Oxidation of Ruddlesden–Popper-Type La2NiO3F2 within Fluoride-Ion Batteries
VL - 33
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
AB - Here we explore the electronic structure of the diiron complex [(dppf)Fe(CO)3]0/+ [10/+; dppf = 1,1′-bis(diphenylphosphino)ferrocene] in two oxidation states by an advanced multitechnique experimental approach. A combination of magnetic circular dichroism, X-ray absorption and emission, high-frequency electron paramagnetic resonance (EPR), and Mössbauer spectroscopies is used to establish that oxidation of 10 occurs on the carbonyl iron ion, resulting in a low-spin iron(I) ion. It is shown that an unequivocal result is obtained by combining several methods. Compound 1+ displays slow spin dynamics, which is used here to study its geometric structure by means of pulsed EPR methods. Surprisingly, these data show an association of the tetrakis[3,5-bis(trifluoromethylphenyl)]borate counterion with 1+.
AU - Winkler, Mario
AU - Schnierle, Marc
AU - Ehrlich, Felix
AU - Mehnert, Kim-Isabelle
AU - Hunger, David
AU - Sheveleva, Alena M.
AU - Burkhardt, Lukas
AU - Bauer, Matthias
AU - Tuna, Floriana
AU - Ringenberg, Mark R.
AU - van Slageren, Joris
ID - 41012
IS - 5
JF - Inorganic Chemistry
KW - Inorganic Chemistry
KW - Physical and Theoretical Chemistry
SN - 0020-1669
TI - Electronic Structure of a Diiron Complex: A Multitechnique Experimental Study of [(dppf)Fe(CO) 3]+/0
VL - 60
ER -
TY - JOUR
AB - Platinum hydride species catalyze a number of interesting organic reactions. However, their reactions typically involve the use of high loadings of noble metal and are difficult to recycle, making them somewhat unsustainable. We have synthesized surface-immobilized Pt–H species via oxidative addition of surface OH groups to Pt(PtBu3)2 (1), a rarely used immobilization technique in surface organometallic chemistry. The hydride species thus made were characterized by infrared, magic-angle spinning nuclear magnetic resonance, and X-ray absorption spectroscopies and catalyzed both olefin isomerization and cycloisomerization of a 1,6 enyne (5) with a high selectivity and low Pt loading.
AU - Maier, Sarah
AU - Cronin, Steve P.
AU - Vu Dinh, Manh-Anh
AU - Li, Zheng
AU - Dyballa, Michael
AU - Nowakowski, Michal
AU - Bauer, Matthias
AU - Estes, Deven P.
ID - 41009
IS - 11
JF - Organometallics
KW - Inorganic Chemistry
KW - Organic Chemistry
KW - Physical and Theoretical Chemistry
SN - 0276-7333
TI - Immobilized Platinum Hydride Species as Catalysts for Olefin Isomerizations and Enyne Cycloisomerizations
VL - 40
ER -
TY - JOUR
AB - The controlled assembly of well-defined planar nanoclusters from molecular precursors is synthetically challenging and often plagued by the predominant formation of 3D-structures and nanoparticles. Herein, we report planar iron hydride nanoclusters from reactions of main group element hydrides with iron(II) bis(hexamethyldisilazide). The structures and properties of isolated Fe4, Fe6, and Fe7 nanoplatelets and calculated intermediates enable an unprecedented insight into the underlying building principle and growth mechanism of iron clusters, metal monolayers, and nanoparticles.
AU - Chakraborty, Uttam
AU - Bügel, Patrick
AU - Fritsch, Lorena
AU - Weigend, Florian
AU - Bauer, Matthias
AU - Jacobi von Wangelin, Axel
ID - 41011
IS - 2
JF - ChemistryOpen
KW - General Chemistry
SN - 2191-1363
TI - Planar Iron Hydride Nanoclusters: Combined Spectroscopic and Theoretical Insights into Structures and Building Principles
VL - 10
ER -
TY - BOOK
ED - Standke, Jan
ED - Topalovic, Elvira
ID - 40920
KW - General Earth and Planetary Sciences
KW - General Environmental Science
SN - 0418-9426
TI - In Krisen erzählen – von Krisen erzählen. Sprachliche, literarische und mediale Dimensionen.
VL - 68
ER -
TY - CHAP
AU - Sackel, Johanna
AU - Wöbse, Anna-Katharina
ED - Torma, Franziska
ID - 40494
SN - 9781474299107
T2 - A Cultural History of the Sea in the Global Age
TI - Networks
VL - 6
ER -
TY - BOOK
ED - Plien, Christian
ED - Topalovic, Elvira
ID - 37092
KW - General Earth and Planetary Sciences
KW - General Environmental Science
SN - 0418-9426
TI - Mehrdeutigkeiten
VL - 68
ER -
TY - CONF
AU - Adelt, Peer
AU - Koppelmann, Bastian
AU - Müller, Wolfgang
AU - Scheytt, Christoph
ID - 23992
T2 - Workshop Methoden und Beschreibungssprachen zur Modellierung und Verifikation von Schaltungen und Systemen (MBMV 2021)
TI - Register and Instruction Coverage Analysis for Different RISC-V ISA Modules
ER -