Hybrid gas -to -particle conversion and chemical vapor deposition for production of high -surface area films.

摘要

A hybrid process, based upon gas-to-particle conversion and chemical vapor deposition, is presented as an alternative technique for producing porous films with the main advantages of solvent-free, low-substrate temperature operation. Starting from solid precursors, nanoparticles were produced in the vapor phase. Downstream of this reaction zone, these nanoparticles were collected via thermophoresis onto a cooled substrate forming a porous film. Initially, alumina (Al2O3) films were produced. Later, multi-component processing was explored by incorporating platinum (Pt) nanoparticles into the Al2O3 matrix leading to the production of Pt/Al 2O3 films by two routes: simultaneous precursor injection processing or by a layer-by-layer approach.;In single component processing, the formation of nanoparticle aggregates was evident within the amorphous Al2O3 films. Aggregates, composed of these particles, are likely held together by relatively weak van der Waals forces leading to the observed poor physical cohesion. In multi-component processing, reasonable control of composition and distribution of species is possible with Pt nanoparticles appearing to be co-agglomerated with alumina. Deposited crystalline Pt nanoparticles may encourage the crystallization of the amorphous Al2O3. Finally, from chemisorption results, the produced sample appears to have potentially greater catalytic activity than a commercially available standard.;A model is in development to study nanoparticle interactions with a gas and deposition occurring in stagnation flow onto the cooled horizontal substrate within the tubular reactor. Using velocity and temperature fields generated from numerical solutions to the Navier-Stokes and energy equations, particle trajectories were calculated from the summation of drag, gravitational, thermophoretic, and Brownian forces. In rectangular coordinates, cooling stage width to reactor diameter ratio, deposition stage temperature, and initial velocity were the primary parameters varied in this study. An optimum balance between thermophoretic and drag forces appears to be the key factor in obtaining high yield and surface uniformity in the films. The results also suggest that Brownian motion is not a significant contributor to deposition under conditions in this study.