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- ItemSelective hydrogenation of fluorinated arenes using rhodium nanoparticles on molecularly modified silica(London : RSC Publ., 2020) Kacem, Souha; Emondts, Meike; Bordet, Alexis; Leitner, WalterThe production of fluorinated cyclohexane derivatives is accomplished through the selective hydrogenation of readily available fluorinated arenes using Rh nanoparticles on molecularly modified silica supports (Rh@Si-R) as highly effective and recyclable catalysts. The catalyst preparation comprises grafting non-polar molecular entities on the SiO2 surface generating a hydrophobic environment for controlled deposition of well-defined rhodium particles from a simple organometallic precursor. A broad range of fluorinated cyclohexane derivatives was shown to be accessible with excellent efficacy (0.05-0.5 mol% Rh, 10-55 bar H2, 80-100 °C, 1-2 h), including industrially relevant building blocks. Addition of CaO as scavenger for trace amounts of HF greatly improves the recyclability of the catalytic system and prevents the risks associated to the presence of HF, without compromising the activity and selectivity of the reaction. © The Royal Society of Chemistry.
- ItemHighly active heterogeneous hydrogenation catalysts prepared from cobalt complexes and rice husk waste(London : RSC Publ., 2022) Unglaube, Felix; Schlapp, Janina; Quade, Antje; Schäfer, Jan; Mejía, EstebanThe utilization and valorization of agricultural waste is a key strategy for the implementation of a sustainable economy to lessen the environmental footprint of human activities on Earth. This work describes the use of rice husk (RH) from agricultural waste to prepare a highly active catalyst for the reduction of nitro compounds. RH was impregnated with various cobalt complexes bearing N-donor ligands, then pyrolyzed and the resulting composite was etched with a base to remove the silica domains. The composition and morphology of the prepared materials were investigated by IR, AAS, ICP-OES, XRD, BET, XPS and SEM technics. The material showed excellent activity and selectivity in the hydrogenation of nitro groups in aromatic and aliphatic substrates. A remarkable selectivity towards nitro groups was found in the presence of various reactive functionalities, including halogens, carbonyls, borates, and nitriles. Apart from their excellent activity and selectivity, these catalysts showed remarkable stability, allowing their easy recovery and multiple reuse without requiring re-activation.
- ItemHigh temperature behavior of rual thin films on piezoelectric CTGS and LGS substrates(Basel : MDPI AG, 2020) Seifert, M.This paper reports on a significant further improvement of the high temperature stability of RuAl thin films (110 nm) on the piezoelectric Ca3TaGa3Si2O14 (CTGS) and La3Ga5SiO14 (LGS) substrates. RuAl thin films with AlN or SiO2 cover layers and barriers to the substrate (each 20 nm), as well as a combination of both were prepared on thermally oxidized Si substrates, which serve as a reference for fundamental studies, and the piezoelectric CTGS, as well as LGS substrates. In somefilms, additional Al layers were added. To study their high temperature stability, the samples were annealed in air and in high vacuum up to 900 °C, and subsequently their cross-sections, phase formation, film chemistry, and electrical resistivity were analyzed. It was shown that on thermally oxidized Si substrates, all films were stable after annealing in air up to 800 °C and in high vacuum up to 900 °C. The high temperature stability of RuAl thin films on CTGS substrates was improved up to 900 °C in high vacuum by the application of a combined AlN/SiO2 barrier layer and up to 800 °C in air using a SiO2 barrier. On LGS, the films were only stable up to 600 °C in air; however, a single SiO2 barrier layer was sufficient to prevent oxidation during annealing at 900 °C in high vacuum.
- ItemPhase formation and high-temperature stability of very thin co-sputtered Ti-Al and multilayered Ti/Al films on thermally oxidized si substrates(Basel : MDPI AG, 2020) Seifert, M.; Lattner, E.; Menzel, S.B.; Oswald, S.; Gemming, T.Ti-Al thin films with a thickness of 200 nm were prepared either by co-sputtering from elemental Ti and Al targets or as Ti/Al multilayers with 10 and 20 nm individual layer thickness on thermally oxidized Si substrates. Some of the films were covered with a 20-nm-thick SiO2 layer, which was used as an oxidation protection against the ambient atmosphere. The films were annealed at up to 800 °C in high vacuum for 10 h, and the phase formation as well as the film architecture was analyzed by X-ray diffraction, cross section, and transmission electron microscopy, as well as Auger electron and X-ray photoelectron spectroscopy. The results reveal that the co-sputtered films remained amorphous after annealing at 600 °C independent on the presence of the SiO2 cover layer. In contrast to this, the γ-TiAl phase was formed in the multilayer films at this temperature. After annealing at 800 °C, all films were degraded completely despite the presence of the cover layer. In addition, a strong chemical reaction between the Ti and SiO2 of the cover layer and the substrate took place, resulting in the formation of Ti silicide. In the multilayer samples, this reaction already started at 600 °C.
- ItemUltrafast laser inscription of asymmetric integrated waveguide 3 dB couplers for astronomical K-band interferometry at the CHARA array(Washington, DC : Soc., 2021) Benoît, Aurélien; Pike, Fraser A.; Sharma, Tarun K.; MacLachlan, David G.; Dinkelaker, Aline N.; Nayak, Abani S.; Madhav, Kalaga; Roth, Martin M.; Labadie, Lucas; Pedretti, Ettore; Brummelaar, Theo A. ten; Scott, Nic; Coudé du Foresto, Vincent; Thomson, Robert R.We present the fabrication and characterization of 3 dB asymmetric directional couplers for the astronomical K-band at wavelengths between 2.0 and 2.4 µm. The couplers were fabricated in commercial Infrasil silica glass using an ultrafast laser operating at 1030 nm. After optimizing the fabrication parameters, the insertion losses of straight single-mode waveguides were measured to be ∼1.2±0.5dB across the full K-band. We investigate the development of asymmetric 3 dB directional couplers by varying the coupler interaction lengths and by varying the width of one of the waveguide cores to detune the propagation constants of the coupled modes. In this manner, we demonstrate that ultrafast laser inscription is capable of fabricating asymmetric 3 dB directional couplers for future applications in K-band stellar interferometry. Finally, we demonstrate that our couplers exhibit an interferometric fringe contrast of >90%. This technology paves the path for the development of a two-telescope K-band integrated optic beam combiner for interferometry to replace the existing beam combiner (MONA) in Jouvence of the Fiber Linked Unit for Recombination (JouFLU) at the Center for High Angular Resolution Astronomy (CHARA) telescope array.
- ItemDesign, simulation and characterization of integrated photonic spectrographs for astronomy: generation-I AWG devices based on canonical layouts(Washington, DC : Soc., 2021) Stoll, Andreas; Madhav, Kalaga V.; Roth, Martin M.We present an experimental study on our first generation of custom-developed arrayed waveguide gratings (AWG) on a silica platform for spectroscopic applications in near-infrared astronomy. We provide a comprehensive description of the design, numerical simulation and characterization of several AWG devices aimed at spectral resolving powers of 15,000-60,000 in the astronomical H-band. We evaluate the spectral characteristics of the fabricated devices in terms of insertion loss and estimated spectral resolving power and compare the results with numerical simulations. We estimate resolving powers of up to 18,900 from the output channel 3-dB transmission bandwidth. Based on the first characterization results, we select two candidate AWGs for further processing by removal of the output waveguide array and polishing the output facet to optical quality with the goal of integration as the primary diffractive element in a cross-dispersed spectrograph. We further study the imaging properties of the processed AWGs with regards to spectral resolution in direct imaging mode, geometry-related defocus aberration, and polarization sensitivity of the spectral image. We identify phase error control, birefringence control, and aberration suppression as the three key areas of future research and development in the field of high-resolution AWG-based spectroscopy in astronomy.
- ItemFormation of intermittent covalent bonds at high contact pressure limits superlow friction on epitaxial graphene(College Park, MD : APS, 2023) Szczefanowicz, Bartosz; Kuwahara, Takuya; Filleter, Tobin; Klemenz, Andreas; Mayrhofer, Leonhard; Bennewitz, Roland; Moseler, MichaelEpitaxial graphene on SiC(0001) exhibits superlow friction due to its weak out-of-plane interactions. Friction-force microscopy with silicon tips shows an abrupt increase of friction by one order of magnitude above a threshold normal force. Density-functional tight-binding simulations suggest that this wearless high-friction regime involves an intermittent sp3 rehybridization of graphene at contact pressure exceeding 10 GPa. The simultaneous formation of covalent bonds with the tip's silica surface and the underlying SiC interface layer establishes a third mechanism limiting the superlow friction on epitaxial graphene, in addition to dissipation in elastic instabilities and in wear processes.
- ItemEfficient suboxide sources in oxide molecular beam epitaxy using mixed metal + oxide charges: The examples of SnO and Ga2O(Melville, NY : AIP Publ., 2020) Hoffmann, Georg; Budde, Melanie; Mazzolini, Piero; Bierwagend, OliverSources of suboxides, providing several advantages over metal sources for the molecular beam epitaxy (MBE) of oxides, are conventionally realized by decomposing the corresponding oxide charge at extreme temperatures. By quadrupole mass spectrometry of the direct flux from an effusion cell, we compare this conventional approach to the reaction of a mixed oxide + metal charge as a source for suboxides with the examples of SnO2 + Sn → 2 SnO and Ga2O3 + 4 Ga → 3 Ga2O. The high decomposition temperatures of the pure oxide charge were found to produce a high parasitic oxygen background. In contrast, the mixed charges reacted at significantly lower temperatures, providing high suboxide fluxes without additional parasitic oxygen. For the SnO source, we found a significant fraction of Sn2O2 in the flux from the mixed charge that was basically absent in the flux from the pure oxide charge. We demonstrate the plasma-assisted MBE growth of SnO2 using the mixed Sn + SnO2 charge to require less activated oxygen and a significantly lower source temperature than the corresponding growth from a pure Sn charge. Thus, the sublimation of mixed metal + oxide charges provides an efficient suboxide source for the growth of oxides by MBE. Thermodynamic calculations predict this advantage for further oxides as well, e.g., SiO2, GeO2, Al2O3, In2O3, La2O3, and Pr2O3 © 2020 Author(s).
- ItemSuitability of binary oxides for molecular-beam epitaxy source materials: A comprehensive thermodynamic analysis(Melville, NY : AIP Publ., 2020) Adkison, Kate M.; Shang, Shun-Li; Bocklund, Brandon J.; Klimm, Detlef; Schlom, Darrell G.; Liu, Zi-KuiWe have conducted a comprehensive thermodynamic analysis of the volatility of 128 binary oxides to evaluate their suitability as source materials for oxide molecular-beam epitaxy (MBE). 16 solid or liquid oxides are identified that evaporate nearly congruently from stable oxide sources to gas species: As2O3, B2O3, BaO, MoO3, OsO4, P2O5, PbO, PuO2, Rb2O, Re2O7, Sb2O3, SeO2, SnO, ThO2, Tl2O, and WO3. An additional 24 oxides could provide molecular beams with dominant gas species of CeO, Cs2O, DyO, ErO, Ga2O, GdO, GeO, HfO, HoO, In2O, LaO, LuO, NdO, PmO, PrO, PuO, ScO, SiO, SmO, TbO, Te2O2, U2O6, VO2, and YO2. The present findings are in close accord with available experimental results in the literature. For example, As2O3, B2O3, BaO, MoO3, PbO, Sb2O3, and WO3 are the only oxides in the ideal category that have been used in MBE. The remaining oxides deemed ideal for MBE awaiting experimental verification. We also consider two-phase mixtures as a route to achieve the desired congruent evaporation characteristic of an ideal MBE source. These include (Ga2O3 + Ga) to produce a molecular beam of Ga2O(g), (GeO2 + Ge) to produce GeO(g), (SiO2 + Si) to produce SiO(g), (SnO2 + Sn) to produce SnO(g), etc.; these suboxide sources enable suboxide MBE. Our analysis provides the vapor pressures of the gas species over the condensed phases of 128 binary oxides, which may be either solid or liquid depending on the melting temperature. © 2020 Author(s).
- ItemEffect of Liquid Hot Water Pretreatment on Hydrolysates Composition and Methane Yield of Rice Processing Residue(Basel : MDPI, 2021) López González, Lisbet Mailin; Heiermann, MonikaLignocellulosic rice processing residue was pretreated in liquid hot water (LHW) at three different temperatures (140, 160, and 180 °C) and two pretreatment times (10 and 20 min) in order to assess its effects on hydrolysates composition, matrix structural changes and methane yield. The concentrations of acetic acid, 5-hydroxymethylfurfural and furfural increased with pretreatment severity (log Ro). The maximum methane yield (276 L kg−1 VS) was achieved under pretreatment conditions of 180 °C for 20 min, with a 63% increase compared to untreated biomass. Structural changes resulted in a slight removal of silica on the upper portion of rice husks, visible predominantly at maximum severity. However, the outer epidermis was kept well organized. The results indicate, at severities 2.48 ≤ log Ro ≤ 3.66, a significant potential for the use of LHW to improve methane production from rice processing residue.