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- ItemHighly selective hydrogenation of amides catalysed by a molybdenum pincer complex : Scope and mechanism(Cambridge : RSC, 2019) Leischner, Thomas; Suarez, Lluis Artús; Spannenberg, Anke; Nova, Ainara; Junge, Kathrin; Nova, Ainara; Beller, MatthiasA series of molybdenum pincer complexes has been shown for the first time to be active in the catalytic hydrogenation of amides. Among the tested catalysts, Mo-1a proved to be particularly well suited for the selective C-N hydrogenolysis of N-methylated formanilides. Notably, high chemoselectivity was observed in the presence of certain reducible groups including even other amides. The general catalytic performance as well as selectivity issues could be rationalized taking an anionic Mo(0) as the active species. The interplay between the amide CO reduction and the catalyst poisoning by primary amides accounts for the selective hydrogenation of N-methylated formanilides. The catalyst resting state was found to be a Mo-alkoxo complex formed by reaction with the alcohol product. This species plays two opposed roles-it facilitates the protolytic cleavage of the C-N bond but it encumbers the activation of hydrogen. This journal is © The Royal Society of Chemistry.
- ItemScalable Functionalization of Optical Fibers Using Atomically Thin Semiconductors(Weinheim : Wiley-VCH Verlag, 2020) Ngo G.Q.; George A.; Schock R.T.K.; Tuniz A.; Najafidehaghani E.; Gan Z.; Geib N.C.; Bucher T.; Knopf H.; Saravi S.; Neumann C.; Lühder T.; Schartner E.P.; Warren-Smith S.C.; Ebendorff-Heidepriem H.; Pertsch T.; Schmidt M.A.; Turchanin A.; Eilenberger F.Atomically thin transition metal dichalcogenides are highly promising for integrated optoelectronic and photonic systems due to their exciton-driven linear and nonlinear interactions with light. Integrating them into optical fibers yields novel opportunities in optical communication, remote sensing, and all-fiber optoelectronics. However, the scalable and reproducible deposition of high-quality monolayers on optical fibers is a challenge. Here, the chemical vapor deposition of monolayer MoS2 and WS2 crystals on the core of microstructured exposed-core optical fibers and their interaction with the fibers’ guided modes are reported. Two distinct application possibilities of 2D-functionalized waveguides to exemplify their potential are demonstrated. First, the excitonic 2D material photoluminescence is simultaneously excited and collected with the fiber modes, opening a novel route to remote sensing. Then it is shown that third-harmonic generation is modified by the highly localized nonlinear polarization of the monolayers, yielding a new avenue to tailor nonlinear optical processes in fibers. It is anticipated that the results may lead to significant advances in optical-fiber-based technologies. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemUltrathin structures derived from interfacially modified polymeric nanocomposites to curb electromagnetic pollution(Cambridge : Royal Society of Chemistry, 2021) Sushmita, Kumari; Formanek, Petr; Fischer, Dieter; Pötschke, Petra; Madras, Giridhar; Bose, SuryasarathiThe use of electronic devices and wireless networks is increasing rapidly, and electromagnetic (EM) pollution remediation remains a challenge. We employed a unique approach to fabricate two ultrathin (approx. 53 μm) multilayered assemblies to address this. By sequentially stacking thin films of polyvinylidene difluoride (PVDF) and polycarbonate (PC) nanocomposites and interfacially locking them with a mutually miscible polymer (PMMA, polymethyl methacrylate), materials with enhanced structural properties and electromagnetic interference (EMI) shielding performance can be designed. Utilizing reduced graphene oxide (rGO) and molybdenum disulfide (MoS2) as a template, ferrite was grown on the surface to design two different nanohybrid structures (rGO–Fe3O4 and MoS2–Fe3O4). PVDF was composited with either rGO–Fe3O4 or MoS2–Fe3O4, and multiwall carbon nanotubes (CNTs) were dispersed in the PC component. As PC and PVDF are immiscible, their poor interface would result in inferior structural properties, which can be challenging in designing EMI shielding materials due to cyclic thermal fatigue. Hence, PMMA is sandwiched to interfacially stitch the components (PC and PVDF) and improve interfacial adhesion. This was confirmed using SEM/EDS and Raman mapping/imaging. The mechanical stability of the multilayered assemblies was characterized using a dynamic mechanical analyzer (DMA), and the storage modulus was found to be as high as 2767 MPa at 40 °C (@constant frequency and strain amplitude), for the multilayered film with rGO–Fe3O4 in PVDF, PMMA as a sandwich layer and CNTs in PC. A typical assembly of 9 multilayers (∼480 μm) with rGO–Fe3O4 in PVDF, and CNTs in PC, and interfacially stitched with PMMA gave rise to a high EMI shield effectiveness (SET) of −26.3 dB @ 26.5 GHz. This unique arrangement of a multilayered assembly suppressed EMI primarily by absorption.
- ItemRoom temperature synthesis of an amorphous MoS2 based composite stabilized by N-donor ligands and its light-driven photocatalytic hydrogen production(London : RSC Publishing, 2015) Niefind, Felix; Djamil, John; Bensch, Wolfgang; Srinivasan, Bikshandarkoil R.; Sinev, Ilya; Grünert, Wolfgang; Deng, Mao; Kienle, Lorenz; Lotnyk, Andriy; Mesch, Maria B.; Senker, Jürgen; Dura, Laura; Beweries, TorstenHerein an entirely new and simple room temperature synthesis of an amorphous molybdenum sulfide stabilized by complexing ammonia and hydrazine is reported. The resulting material exhibits an outstanding activity for the photocatalytic hydrogen evolution driven by visible light. It is chemically stable during the reaction conditions of the photocatalysis and shows unusual thermal stability up to 350 °C without crystallization. The new material is obtained by a reaction of solid ammonium tetrathiomolybdate and gaseous hydrazine. In the as-prepared state Mo atoms are surrounded by μ2-briding S2−, NH3 and hydrazine, the latter being coordinated to Mo(IV) in a bridging or side-on mode. Heating at 450 °C or irradiation with an electron beam generates nanosized crystalline MoS2 slabs. The two modes for crystallization are characterized by distinct mechanisms for crystal growth. The stacking of the slabs is low and the material exhibits a pronounced turbostratic disorder. Heat treatment at 900 °C yields more ordered MoS2 but structural disorder is still present. The visible-light driven hydrogen evolution experiments evidence an outstanding performance of the as-prepared sample. The materials were thoroughly characterized by optical spectroscopy, chemical analysis, in situ HRTEM, XRD, 1H and 15N solid-state NMR, XPS, and thermal analysis.