Advanced modeling of nanoparticle nucleation: towards the simulation of particle synthesis

Abstract

Nanotechnology holds a lot of promise for the discovery of new phenomena, and many of the envisioned processes involve nanoparticles. These particles are found in chemical sensors, drug targeting and delivery, and one important application is motivated by the need of clean renewable energy sources. Gas-to-particle conversion in the form of homogeneous nucleation within flow systems plays a significant role in a variety of natural and industrial processes of nanoparticle synthesis. In this work, nucleation processes of several metal materials and dibutyl phthalate (DBP) nanoparticles in laminar and turbulent flows are investigated via direct numerical simulations (DNS). The flows consist of condensing vapor diluted in argon or nitrogen issuing into a cooler particle-free stream. DNS facilitates probing the interactive effects of fluid dynamics and nucleation in an accurate manner. The fluid, thermal and chemical fields are obtained by solving the Navier-Stokes, enthalpy, and mass transport equations. Nucleation is simulated via calibrated classical homogeneous nucleation models. Recently developed size dependent surface tension model offers increased accuracy in predicting metal particle nucleation. This approach is attractive in that it promises to be more accurate than the classical nucleation theory while maintaining much of its simplicity when coupling with fluid dynamics. The effects of turbulence on metal nucleation are also studied using fully resolved DNS to elucidate the effects of different stages of fluid mixing on metal particle nucleation. The effects of nucleation on fluid dynamics are investigated via DNS of DBP nucleation within both laminar and turbulent jet flows. The simulations provide a demonstration of how heat release affects the interactions of fluid dynamics and nucleation at different Reynolds numbers and particle formation rates. The results provide insights into the interaction of fluid, thermal transport and nanoparticle nucleation in various flows, which stimulate development of models that will allow engineers to optimize the fluid and thermal environments for industrial nanoparticle production. For brevity, specific conclusions are provided in each chapter.