Abstract:In this contribution, we report the successful preparation of supported metal catalysts using dendrimer-encapsulated Pt nanoparticles as metal precursors. Polyamidoamine (PAMAM) dendrimers were first used to template and stabilize Pt nanoparticles prepared in solution. These dendrimer-encapsulated nanoparticles were then deposited onto a commercial high surface area silica support and thermally activated to remove the organic dendrimer. The resulting materials are active oxidation and hydrogenation catalysts. The effects of catalyst preparation and activation on activity for toluene hydrogenation and CO oxidation catalysis are discussed.

The desorption kinetics for Ar, Kr, Xe, N2, O2, CO, methane, ethane, and propane from graphene-covered Pt(111) and amorphous solid water (ASW) surfaces are investigated using temperature-programmed desorption (TPD). The TPD spectra for all of the adsorbates from graphene have well-resolved first, second, third, and multilayer desorption peaks. The alignment of the leading edges is consistent the zero-order desorption for all of the adsorbates. An Arrhenius analysis is used to obtain desorption energies and prefactors for desorption from graphene for all of the adsorbates. In contrast, the leading desorption edges for the adsorbates from ASW do not align (for coverages < 2 ML). The nonalignment of TPD leading edges suggests that there are multiple desorption binding sites on the ASW surface. Inversion analysis is used to obtain the coverage dependent desorption energies and prefactors for desorption from ASW for all of the adsorbates.

Two sets of silicon (Si) heterojunctions with either Au or PEDOT:PSS contacts have been prepared to compare interfacial majority carrier charge transfer processes at Si/metal and Si/polymer heterojunctions. Current-voltage (J-V) responses at a range of temperatures, wavelength-dependent internal quantum yields, and steady-state J-V responses under illumination for these devices are reported. The cumulative data suggest that the velocity of majority carrier charge transfer, vn, is several orders of magnitude smaller at n-Si/PEDOT:PSS contacts than at n-Si/Au junctions, resulting in superior photoresponse characteristics for these inorganic/organic heterojunctions.

High surface area, porous titanium carbide films have been synthesized at room temperature via reactive ballistic deposition (RBD). X-ray diffraction and X-ray photoelectron spectroscopy show that evaporative deposition of titanium in an ethylene ambient environment allows for low temperature (35 °C) synthesis of nanocrystalline titanium carbide, a material which typically requires high processing temperatures to produce. Angle-dependent RBD allows for the controlled tuning of TiC nanostructure and porosity where changing the deposition angle from near normal incidence (13°) to more glancing angles (50−85°) changes the film morphology from relatively nonporous, dense TiC to a continuous, reticulated TiC and finally to discrete, nanocolumnar TiC. The influence of the deposition angle on TiC optical constants, porosity, specific surface area, and the pore size distribution has been investigated using hybrid quartz crystal microbalance and ellipsometric porosimetry. Notably, TiC films deposited at 35 °C at an angle of 70° have a specific surface area of 710 m2·g−1 and a mean Kelvin radius of 1.8 nm, making them attractive materials for application in catalysis, energy conversion, and storage.