
This dissertation uses multi-million atom molecular dynamics simulations to determine the key mechanisms which control the oxidation of aluminum nanoparticles (ANPs) due to uniform heating. The primary simulation studied is the oxidation of a 46 nm ANP uniformly heated to 1100 K (the melting temperature of aluminum metal is 933 K). In this system, 3 stages are identified, corresponding to simulation times of 0 to 50 ps (Stage 1), 60 to 110 ps (Stage 2), and 120 to 1000 ps (Stage 3). Radial analysis, fragment analysis, and other simulation tools are used to determine the controlling mechanisms in each stage, as well as determining the cause of each stage transition. Stage 1, initiated by the ANP temperature exceeding the melting temperature of the aluminum core, is seen to be a confined burning stage. Oxygen penetrating from the core-shell interface reacts exothermically with the core metal, releasing local heat. When this heating drives the local temperature of the shell to exceed the melting temperature of alumina (the shell), a sudden increase in the number of oxidation reactions is seen. The development of asymmetry in the shell and increased uptake of oxygen from the exterior also support the conclusion that melting of the shell initiates Stage 2. Local heating continues until the shell temperature reaches a critical temperature (T = 3000 K), at which point aluminum atom ejections from the exterior of the shell into the surrounding oxygen begin. These ejections lead to direct oxidation outside the ANP and the formation of oxygen-rich clusters. Both internal and external oxidation continue throughout the remainder of Stage 3, leading to complete oxidation of the particle.
Physics (degree program), Doctor of Philosophy (degree), College of Letters, Arts and Sciences (school)
Physics (degree program), Doctor of Philosophy (degree), College of Letters, Arts and Sciences (school)
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