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- 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.
- 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.
- 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.