Interstellar dust particles (IDPs) constitute most of the solid matter in the universe. Large quantities of IDPs are also present in the Solar System and fall on Earth. IDPs are also of interest as they can catalyze astrochemical reactions and prebiotic synthesis, and their organic contents are believed to have contributed to the origins of life. Their chemical composition is similar to carbonaceous chondrite comets, asteroids and meteorites. The IDPs are microporous web-like aggregates of 10-100 nm phyllosilicate particles with morphologies similar to particles produced by the Laser Vaporization Controlled Condensation (LVCC) method. IDPs are available only as microscopic samples, and simulated IDPs are needed to study their chemical and catalytic effects. To produce such simulated IDPs, we formed nanoparticles from carbonaceous chondrite meteorites by LVCC processing. The compositions, morphologies, particle size distribution, FTIR spectra, and catalytic properties of the meteorite-based nanoparticles were investigated and compared with the original meteorite materials and reference minerals.
We report the vapor phase synthesis and characterization of supported Pd, Au and unsupported bimetallic nanoparticle catalysts for CO oxidation. The approach utilized in the present work is based on the laser vaporization/controlled condensation technique which uniquely combines the features of pulsed laser vaporization with the controlled condensation process from the vapor phase to synthesize nanoparticle catalysts of controlled size and composition. The results indicate that supported Pd/CeO2, Au/CeO2, and unsupported bimetallic CuPd, CuAu, and AuPd nanoparticle catalysts exhibit excellent activity for CO oxidation. The significance of the current method lies mainly in its simplicity, flexibility and the control of the different factors that determine the activity of the nanoparticle catalysts.
The laser vaporization controlled condensation (LVCC) technique coupled with a differential mobility analyzer (DMA) is used to synthesize size-selected alloy nanoparticles and nanoparticle catalyst systems. The formation of Au–Ag alloy nanoparticles is concluded from the observation of only one plasmon band. The maximum of the plasmon absorption is found to vary linearly with the gold mole fraction. For the Au–Pd system, the XRD data confirms the formation of the alloy nanoparticles with no evidence of any of the pure components. The Au/CeO2 nanoparticle catalyst prepared by the LVCC method is a promising catalyst for low temperature CO oxidation due to its high activity and stability.
In this paper, we demonstrate that laser vaporization of metals in the presence of a small concentration of butadiene vapor leads to the polymerization of butadiene and incorporation of the metal nanoparticles within the polymer matrix. The metal nanocomposites are characterized by electron microscopy, X-ray diffraction and EDX. The results from high pressure mass spectrometry indicate that multiple additions of butadiene molecules on the metal cations Fe+, Ni+ and Pt+, generated by laser vaporization, take place at room temperature thus providing an efficient means of initiating further polymerization reactions. The Pt+ reactions show extensive fragmentations and elimination steps generating hydrocarbon ions. The laser vaporization/polymerization method provides the ability to encapsulate several different metals or metal oxides which undoubtedly will play a significant role in tuning the various properties of the polymer composites.
Dust particles and their interaction with gases play important roles in star formation and in solar nebulae. Appropriate model dust grains are needed for the laboratory simulation of gas-grain interactions. Nanoparticles formed from carbonaceous meteorites may be particularly suitable, as these particles are formed from materials that were formed originally from interstellar/nebula dust. Extending our previous studies with grounded meteorite powders, we demonstrate here the production of nanoparticles formed from meteorites using the laser desorption/controlled condensation method developed in our laboratory. The product nanoparticle aggregates have porous, web-like morphologies similar to interstellar dust grains, indicating that they can present large specific surface areas for gas/grain interactions. In this paper, we present polarisation modulation reflection-absorption infrared spectra (PM-RAIRS) of supported thin films and compare these spectra with the known silicate bands in the spectra of interstellar dust recorded during the ISO mission. We also report an ultrahigh vacuum (UHV) temperature programmed desorption (TPD) study of the adsorption of CO on the supported nanoparticle films. The latter allow us to estimate the CO binding energy on the meteorite nanoparticles as 13.5 +/- 3.0 kJ mol(-1), cf. a value of 9.8 +/- 0.2 kJ mol(-1) for CO binding to a water ice substrate. Such thermochemical data can be useful for computational modelling of gas-grain interactions under the diverse conditions in interstellar clouds and solar nebulae.
A new class of nanoparticle filaments and tree-like aggregates is assembled by the influence of an electric field during the synthesis of metallic, intermetallic, silicon, and carbon nanoparticles from the vapor phase. Enormous electrostatic aggregation due to dipole forces is observed between the nanoparticles to form chain filaments, and between the chain filaments to form tree-like fibers. The filaments and tree-like fibers can grow to lengths exceeding several centimeters. The filaments display stretch and contraction properties depending on the strength of the applied field.
The critical supersaturations and isothermal homogeneous nucleation rates of dodecane, hexadecane, and octadecane vapors have been measured over wide temperature ranges (e.g., 285-340 K) using an upward thermal diffusion cloud chamber. Dodecane shows the best agreement between the experiment and the classical nucleation theory. Hexadecane and octadecane exhibit critical supersaturations lower than those predicted by the theory. All three compounds show increasing deviation from theory with decreasing temperature. This trend is also observed in the measured nucleation rates where the predictions of the theory at lower temperatures are shifted to much lower values compared to the experimental data. Temperature dependence correction factors to the calculated rates have been evaluated based on the experimental rates of the studied higher alkanes. The classical theory predicts the correct supersaturation dependence of the nucleation rates of these compounds. Analysis of the supersaturation dependence of the nucleation rate of octadecane indicates that the critical cluster contains 30-35 molecules at the nucleation temperatures of 315-340 K. The classical theory predicts smaller nucleus size as a result of the overestimation of the supersaturation corresponding to the measured nucleation rate.