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- ItemCobalt pincer complexes for catalytic reduction of nitriles to primary amines(London : RSC Publ., 2019) Schneekönig, Jacob; Tannert, Bianca; Hornke, Helen; Beller, Matthias; Junge, KathrinVarious cobalt pincer type complexes 1-6 were applied for the catalytic hydrogenation of nitriles to amines. Among these, catalyst 4 is the most efficient, allowing the reduction of aromatic as well as aliphatic nitriles in moderate to excellent yields. © 2019 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.
- ItemTuning the magneto-optical response of TbPc2 single molecule magnets by the choice of the substrate(London [u.a.] : RSC, 2015) Robaschik, Peter; Fronk, Michael; Toader, Marius; Klyatskaya, Svetlana; Ganss, Fabian; Siles, Pablo F.; Schmidt, Oliver G.; Albrecht, Manfred; Hietschold, Michael; Ruben, Mario; Zahn, Dietrich R.T.; Salvan, GeorgetaIn this work, we investigated the magneto-optical response of thin films of TbPc2 on substrates which are relevant for (spin) organic field effect transistors (SiO2) or vertical spin valves (Co) in order to explore the possibility of implementing TbPc2 in magneto-electronic devices, the functionality of which includes optical reading. The optical and magneto-optical properties of TbPc2 thin films prepared by organic molecular beam deposition (OMBD) on silicon substrates covered with native oxide were investigated by variable angle spectroscopic ellipsometry (VASE) and magneto-optical Kerr effect (MOKE) spectroscopy at room temperature. The magneto-optical activity of the TbPc2 films can be significantly enhanced by one to two orders of magnitude upon changing the molecular orientation (from nearly standing molecules on SiO2/Si substrates to nearly lying molecules on perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) templated SiO2/Si substrates) or by using metallic ferromagnetic substrates (Co).
- ItemOn the growth of Co-doped BaFe2As2 thin films on CaF2(Bristol : IOP Publ., 2019) Langer, Marco; Meyer, Sven; Ackermann, Kai; Grünewald, Lukas; Kauffmann-Weiss, Sandra; Aswartham, Saicharan; Wurmehl, Sabine; Hänisch, Jens; Holzapfel, BernhardThe competition between phase formation of BaF2 and Ba(Fe1-xCox)2As2 on CaF2 single crystals has been analysed. Ba(Fe0.92Co0.08)2As2 thin films have been deposited by pulsed laser deposition. X-ray diffraction, atomic force microscopy and scanning electron microscopy studies have revealed that the formation of secondary phases and misorientations as well as the growth modes of the Ba(Fe0.92Co0.08)2As2 thin films strongly depend on the growth rate. At high growth rates, formation of BaF2 is suppressed. The dependency of the Ba(Fe0.92Co0.08)2As2 lattice parameters supports the idea of fluorine diffusion into the crystal structure upon suppression of BaF2 formation similar as was proposed for FeSe1-xTex thin films on CaF2. Furthermore, a growth mode transition from a layer growth mechanism to a three-dimensional growth mode at high supersaturation has been found, suggesting similarities between the growth mechanism of iron-based superconductors and high-T c cuprate thin films. © 2019 Published under licence by IOP Publishing Ltd.
- ItemUltra-small cobalt nanoparticles from molecularly-defined Co-salen complexes for catalytic synthesis of amines(Cambridge : RSC, 2020) Senthamarai, Thirusangumurugan; Chandrashekhar, Vishwas G.; Gawande, Manoj B.; Kalevaru, Narayana V.; Zbořil, Radek; Kamer, Paul C.J.; Jagadeesh, Rajenahally V.; Beller, MatthiasWe report the synthesis of in situ generated cobalt nanoparticles from molecularly defined complexes as efficient and selective catalysts for reductive amination reactions. In the presence of ammonia and hydrogen, cobalt-salen complexes such as cobalt(ii)-N,N′-bis(salicylidene)-1,2-phenylenediamine produce ultra-small (2-4 nm) cobalt-nanoparticles embedded in a carbon-nitrogen framework. The resulting materials constitute stable, reusable and magnetically separable catalysts, which enable the synthesis of linear and branched benzylic, heterocyclic and aliphatic primary amines from carbonyl compounds and ammonia. The isolated nanoparticles also represent excellent catalysts for the synthesis of primary, secondary as well as tertiary amines including biologically relevant N-methyl amines. This journal is © The Royal Society of Chemistry.
- ItemHigh-defect hydrophilic carbon cuboids anchored with Co/CoO nanoparticles as highly efficient and ultra-stable lithium-ion battery anodes(Cambridge : Royal Society of Chemistry, 2016) Sun, Xiaolei; Hao, Guang-Ping; Lu, Xueyi; Xi, Lixia; Liu, Bo; Si, Wenping; Ma, Chuansheng; Liu, Qiming; Zhang, Qiang; Kaskel, Stefan; Schmidt, Oliver G.We propose an effective strategy to engineer a unique kind of porous carbon cuboid with tightly anchored cobalt/cobalt oxide nanoparticles (PCC–CoOx) that exhibit outstanding electrochemical performance for many key aspects of lithium-ion battery electrodes. The host carbon cuboid features an ultra-polar surface reflected by its high hydrophilicity and rich surface defects due to high heteroatom doping (N-/O-doping both higher than 10 atom%) as well as hierarchical pore systems. We loaded the porous carbon cuboid with cobalt/cobalt oxide nanoparticles through an impregnation process followed by calcination treatment. The resulting PCC–CoOx anode exhibits superior rate capability (195 mA h g−1 at 20 A g−1) and excellent cycling stability (580 mA h g−1 after 2000 cycles at 1 A g−1 with only 0.0067% capacity loss per cycle). Impressively, even after an ultra-long cycle life exceeding 10 000 cycles at 5 A g−1, the battery can recover to 1050 mA h g−1 at 0.1 A g−1, perhaps the best performance demonstrated so far for lithium storage in cobalt oxide-based electrodes. This study provides a new perspective to engineer long-life, high-power metal oxide-based electrodes for lithium-ion batteries through controlling the surface chemistry of carbon host materials.
- ItemAnalyzer-free, intensity-based, wide-field magneto-optical microscopy(Melville, NY : American Inst. of Physics, 2021) Schäfer, Rudolf; Oppeneer, Peter M.; Ognev, Alexey; Samardak, Alexander; Soldatov, Ivan V.In conventional Kerr and Faraday microscopy, the sample is illuminated with plane-polarized light, and a magnetic domain contrast is generated by an analyzer making use of the Kerr or Faraday rotation. Here, we demonstrate possibilities of analyzer-free magneto-optical microscopy based on magnetization-dependent intensity modulations of the light. (i) The transverse Kerr effect can be applied for in-plane magnetized material, as demonstrated for an FeSi sheet. (ii) Illuminating that sample with circularly polarized light leads to a domain contrast with a different symmetry from the conventional Kerr contrast. (iii) Circular polarization can also be used for perpendicularly magnetized material, as demonstrated for garnet and ultrathin CoFeB films. (iv) Plane-polarized light at a specific angle can be employed for both in-plane and perpendicular media. (v) Perpendicular light incidence leads to a domain contrast on in-plane materials that is quadratic in the magnetization and to a domain boundary contrast. (vi) Domain contrast can even be obtained without a polarizer. In cases (ii) and (iii), the contrast is generated by magnetic circular dichroism (i.e., differential absorption of left- and right-circularly polarized light induced by magnetization components along the direction of light propagation), while magnetic linear dichroism (differential absorption of linearly polarized light induced by magnetization components transverse to propagation) is responsible for the contrast in case (v). The domain-boundary contrast is due to the magneto-optical gradient effect. A domain-boundary contrast can also arise by interference of phase-shifted magneto-optical amplitudes. An explanation of these contrast phenomena is provided in terms of Maxwell-Fresnel theory. © 2021 Author(s).
- ItemPhononic-magnetic dichotomy of the thermal Hall effect in the Kitaev material Na2 Co2 TeO6(College Park, MD : APS, 2023) Gillig, Matthias; Hong, Xiaochen; Wellm, Christoph; Kataev, Vladislav; Yao, Weiliang; Li, Yuan; Büchner, Bernd; Hess, ChristianThe quest for a half-quantized thermal Hall effect of a Kitaev system represents an important tool to probe topological edge currents of emergent Majorana fermions. Pertinent experimental findings for α-RuCl3 are, however, strongly debated, and it has been argued that the thermal Hall signal stems from phonons or magnons rather than from Majorana fermions. Here, we investigate the thermal Hall effect of the Kitaev candidate material Na2Co2TeO6, and we show that the measured signal emerges from at least two components, phonons and magnetic excitations. This dichotomy results from our discovery that the longitudinal and transversal heat conductivities share clear phononic signatures, while the transversal signal changes sign upon entering the low-temperature, magnetically ordered phase. Our results demonstrate that uncovering a genuinely quantized magnetic thermal Hall effect in Kitaev topological quantum spin liquids such as α-RuCl3 and Na2Co2TeO6 requires disentangling phonon vs magnetic contributions, including potentially fractionalized excitations such as the expected Majorana fermions.
- ItemThree-Dimensional Cobalt Hydroxide Hollow Cube/Vertical Nanosheets with High Desalination Capacity and Long-Term Performance Stability in Capacitive Deionization([Beijing] : China Association for Science and Technology, 2021) Xiong, Yuecheng; Yu, Fei; Arnold, Stefanie; Wang, Lei; Presser, Volker; Ren, Yifan; Ma, JieFaradaic electrode materials have significantly improved the performance of membrane capacitive deionization, which offers an opportunity to produce freshwater from seawater or brackish water in an energy-efficient way. However, Faradaic materials hold the drawbacks of slow desalination rate due to the intrinsic low ion diffusion kinetics and inferior stability arising from the volume expansion during ion intercalation, impeding the engineering application of capacitive deionization. Herein, a pseudocapacitive material with hollow architecture was prepared via template-etching method, namely, cuboid cobalt hydroxide, with fast desalination rate (3.3 mg (NaCl)·g-1 (h-Co(OH)2)·min-1 at 100 mA·g-1) and outstanding stability (90% capacity retention after 100 cycles). The hollow structure enables swift ion transport inside the material and keeps the electrode intact by alleviating the stress induced from volume expansion during the ion capture process, which is corroborated well by in situ electrochemical dilatometry and finite element simulation. Additionally, benefiting from the elimination of unreacted bulk material and vertical cobalt hydroxide nanosheets on the exterior surface, the synthesized material provides a high desalination capacity ( mg (NaCl)·g-1 (h-Co(OH)2) at 30 mA·g-1). This work provides a new strategy, constructing microscale hollow faradic configuration, to further boost the desalination performance of Faradaic materials.