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Bernd Spliethoff

Publications and source records attributed to Bernd Spliethoff.

12 recordsLinked to original sources

Laser-assisted synthesis of Au-Ag alloy nanoparticles in solution.

By using laser-induced heating, we prepared Au-Ag nanoalloys via three different procedures: (i) mixture of Au nanoparticles and Ag(+) ions irradiated by a 532 nm laser, (ii) mixture of Au and Ag nanoparticles irradiated by a 532 nm laser, and (iii) mixture of Au and Ag nanoparticles irradiated by a 355 nm laser. Procedure i is advantageous for the production of spherical alloy nanoparticles; in procedures ii and iii, nanoalloys with a sintered structure have been obtained. The morphology of the obtained nanoalloys depends not only on the laser wavelength but also on the concentration of nanoparticles in the initial mixture. When the total concentration of Ag and Au nanoparticles in the mixture is increased, large-scale interlinked networks have been observed upon laser irradiation. It is expected that this selective heating strategy can be extended to prepare other bi- or multi-metallic nanoalloys.

Alloys↗

Support effect in high activity gold catalysts for CO oxidation.

In this work, we present a detailed study concerning the evaluation of the metal-support interaction in high activity gold catalysts for CO oxidation. Using the colloidal deposition method, model catalysts were prepared, which allow the isolation of the effect of the support on the catalytic activity. Prefabricated gold particles were thus deposited on different support materials. Since the deposition process did not change the particle sizes of the gold particles, only the influence of the support could be studied. TiO2, Al2O3, ZrO2, and ZnO were used as support materials. Catalytic tests and high resolution transmission electron microscopy clearly show that the support contributes to the activity. However, our results are not in line with the distinction between active and passive supports based on the semiconducting properties of the oxidic material. The most active catalysts were obtained with TiO2 and Al2O3, while ZnO and ZrO2 gave substantially less active catalysts. Furthermore, the effect of other important parameters on the catalytic activity (i.e., particles size distribution, calcination temperature, and aging time for a Au/TiO2 catalyst) has also been studied. Using this preparation route, the catalysts show high-temperature stability, size dependent activity, and a very good long-term stability.

Journal Article↗

Hierarchically structured monolithic silicalite-1 consisting of crystallized nanoparticles and its performance in the Beckmann rearrangement of cyclohexanone oxime.

In this study, we present a synthetic pathway for the fabrication of self-supporting zeolite monoliths consisting of crystallized nanoparticles. A resorcinol-formaldehyde-based organic aerogel is used as a template, and silicalite-1 is used as the zeolite example. The silicalite-1 monoliths obtained consist of individual well-defined zeolite nanocrystals with sizes of 30-40 nm. The monoliths exhibit a high mechanical stability and have hierarchical porosity, with micropores within the zeolite particles, a mesopore system formed by the packing of the nanoparticles, and a macropore system on the monolith level. Such monolithic zeolites show high selectivity typically above 80% to epsilon-caprolactam combined with a high rate of reaction of 0.46 g(caprolactame)/(g(catalyst).h) in the Beckmann rearrangement of cyclohexanone oxime.

Carbon↗

Sol-gel synthesis of a multifunctional, hierarchically porous silica/apatite composite.

In this study, a degradable, hierarchically porous silica/apatite composite material is developed from a simple low-temperature synthesis. Mesoporosity is induced in the silica portion by the use of supramolecular templating. The template is further removed by calcination. Firstly, hydroxyapatite is synthesized through a sol-gel method at near room temperature conditions. After the mineralization process, the crystal surface is coated with a mesoporous silica matrix using the templates already present in the bulk solution. The material is characterized by XRD, N(2)-sorption, FT-IR, SEM/EDS, and TEM. The coating layer is distributed fairly homogeneously over the apatite surface and the coating thickness is easily adjustable and dependent on the amount of added silica precursor. The hybrid material is shown to efficiently induce calcium phosphate formation under in vitro conditions and simultaneously work as a carrier system for drugs.

Bone Substitutes↗

Synthesis and characterization of nanocast silica NCS-1 with CMK-3 as a template.

Nanocast silica (NCS-1) was synthesized by a casting process by employing the mesoporous carbon CMK-3 (the replica of SBA-15) as a template, tetraethoxysilane (TEOS) as the silica source, and hydrochloric acid (HCl) as the catalyst. The ordered carbon template was removed by employing different methods, such as calcination, thermal treatment followed by calcination, and controlled combustion. According to XRD and TEM characterization, NCS-1 exhibits an ordered structure with hexagonal symmetry and retains the morphology of the original SBA-15 used for the synthesis of CMK-3 over two replication steps on the nanometer scale. This demonstrates the well-connected porosity in CMK-3 type carbon, which can be used as a mold to synthesize mesostructured materials. The nitrogen adsorption isotherms generally show type IV shape, indicating mesoporous characteristics. The structure of NCS-1 is strongly influenced by variables of the nanocasting process, such as the loading amount of silica, hydrolysis temperature, and carbon removal methods. The surface area, pore size, and pore volume of NCS-1 can be tuned to a certain range by varying these parameters.

Journal Article↗

Highly stable carbon-protected cobalt nanoparticles and graphite shells.

The fabrication of carbon-shell protected cobalt nanoparticles and hollow graphitic shells has been achieved via a pyrolysis process by using monodispersed cobalt nanoparticles as a template. These materials are mesoporous and highly stable under strong acidic and basic conditions.

Journal Article↗

On the nature of the 'heterogeneous' catalyst: nickel-on-charcoal.

Results from aromatic aminations and Kumada couplings, together with spectroscopic analyses (TEM, EDX, ICP-AES, React-IR), reveal that catalysis using nickel-on-charcoal (Ni/C) is most likely of a homogeneous rather than heterogeneous nature. In the course of a reaction with Ni/C, nickel bleed from the support was calculated to be as high as 78%. However, the existence of an equilibrium for this homogeneous species between nickel located inside vs outside the pore system of charcoal strongly favors the former, thus leaving only traces of metal detectable in solution. This accounts for virtually complete recovery of nickel on the charcoal following filtration of a reaction mixture and allows for recycling of the catalyst. TEM and EDX data were used to explain different reactivity profiles of Ni/C, which depended upon the method of reduction used to convert Ni(II)/C to Ni(0) as well as the level of nickel loading on the support.

Amination↗