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 -
TY - JOUR
AU - Steinhoff, Lena
AU - Zondag, Marcellis M.
ID - 41313
JF - Journal of Business Research
KW - Marketing
SN - 0148-2963
TI - Loyalty programs as travel companions: Complementary service features across customer journey stages
VL - 129
ER -
TY - BOOK
ED - Bürgel, Christoph
ED - Koch, Corinna
ED - Schlaak, Claudia
ED - Visser, Judith
ED - Heiderich, Jens
ID - 41333
TI - Zeitschrift für Romanische Sprachen und ihre Didaktik
ER -
TY - GEN
ID - 41283
TI - Konstruktionen und Konstruktionslernen
ER -
TY - BOOK
ED - Bürgel, Christoph
ED - Koch, Corinna
ED - Schlaak, Claudia
ED - Visser, Judith
ID - 41332
TI - Zeitschrift für Romanische Sprachen und ihre Didaktik
ER -
TY - CONF
AU - Kruse, Stephan
AU - Bahmanian, Meysam
AU - Kneuper, Pascal
AU - Kress, Christian
AU - Kurz, Heiko G.
AU - Schneider, Thomas
AU - Scheytt, Christoph
ID - 23995
T2 - The 17th European Radar Conference
TI - Phase Noise Investigation for a Radar System with Optical Clock Distribution
ER -
TY - JOUR
AU - Wojtaszek, Klaudia
AU - Błachucki, Wojciech
AU - Tyrała, Krzysztof
AU - Nowakowski, Michał
AU - Zaja̧c, Marcin
AU - Stȩpień, Joanna
AU - Jagodziński, Paweł
AU - Banaś, Dariusz
AU - Stańczyk, Wiktoria
AU - Czapla-Masztafiak, Joanna
AU - Kwiatek, Wojciech M.
AU - Szlachetko, Jakub
AU - Wach, Anna
ID - 41326
IS - 1
JF - The Journal of Physical Chemistry A
KW - Physical and Theoretical Chemistry
SN - 1089-5639
TI - Determination of Crystal-Field Splitting Induced by Thermal Oxidation of Titanium
VL - 125
ER -
TY - JOUR
AB - Social robots have emerged as a new digital technology that is increasingly being implemented in the educational landscape. While social robots could be deployed to assist young children with their learning in a variety of different ways, the typical approach in educational practices is to supplement the learning process rather than to replace the human caregiver, e.g., the teacher, parent, educator or therapist. When functioning in the role of an educational assistant, social robots will likely constitute a part of a triadic interaction with the child and the human caregiver. Surprisingly, there is little research that systematically investigates the role of the caregiver by examining the ways in which children involve or check in with them during their interaction with another partner—a phenomenon that is known as social referencing. In the present study, we investigated social referencing in the context of a dyadic child–robot interaction. Over the course of four sessions within our longitudinal language-learning study, we observed how 20 pre-school children aged 4–5 years checked in with their accompanying caregivers who were not actively involved in the language-learning procedure. The children participating in the study were randomly assigned to either an interaction with a social robot or a human partner. Our results revealed that all children across both conditions utilized social referencing behaviors to address their caregiver. However, we found that the children who interacted with the social robot did so significantly more frequently in each of the four sessions than those who interacted with the human partner. Further analyses showed that no significant change in their behavior over the course of the sessions could be observed. Findings are discussed with regard to the caregiver's role during children's interactions with social robots and the implications for future interaction design.
AU - Tolksdorf, Nils F.
AU - Crawshaw, Camilla E.
AU - Rohlfing, Katharina
ID - 37185
JF - Frontiers in Education
KW - Education
SN - 2504-284X
TI - Comparing the Effects of a Different Social Partner (Social Robot vs. Human) on Children's Social Referencing in Interaction
VL - 5
ER -
TY - JOUR
AU - Rohlfing, Katharina
AU - Mertens, Ulrich
ID - 37184
JF - Frontiers in Psychology
TI - Progressive Reduction of Iconic Gestures Contributes to School-Aged Children’s Increased Word Production
ER -
TY - JOUR
AB - Temperamental traits can decisively influence how children enter into social interaction with their environment. Yet, in the field of child–robot interaction, little is known about how individual differences such as shyness impact on how children interact with social robots in educational settings. The present study systematically assessed the temperament of 28 preschool children aged 4–5 years in order to investigate the role of shyness within a dyadic child–robot interaction. Over the course of four consecutive sessions, we observed how shy compared to nonshy children interacted with a social robot during a word-learning educational setting and how shyness influenced children’s learning outcomes. Overall, results suggested that shy children not only interacted differently with a robot compared to nonshy children, but also changed their behavior over the course of the sessions. Critically, shy children interacted less expressively with the robot in general. With regard to children’s language learning outcomes, shy children scored lower on an initial posttest, but were able to close this gap on a later test, resulting in all children retrieving the learned words on a similar level. When intertest learning gain was considered, regression analyses even confirmed a positive predictive role of shyness on language learning gains. Findings are discussed with regard to the role of shyness in educational settings with social robots and the implications for future interaction design.
AU - Tolksdorf, Nils Frederik
AU - Viertel, Franziska E.
AU - Rohlfing, Katharina J.
ID - 24899
JF - Frontiers in Robotics and AI
SN - 2296-9144
TI - Do Shy Preschoolers Interact Differently When Learning Language With a Social Robot? An Analysis of Interactional Behavior and Word Learning
ER -
TY - CHAP
AU - Heidgen, Michael
ID - 41375
T2 - Metzler Lexikon literarischer Symbole
TI - Wurzel
ER -