karen01
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- TL;DR Summary
- Recoil of 224Ra->220Rn in a UO3 aerogel likely typically penetrates 1 or more pores before coming to rest in the matrix, but how to model diffusion rate changes due to the track damage?
I'm working on a theoretical analysis of a thin 232U UO3 aerogel layer (5-20nm feature size, granular, crystalline, ~98% porosity) in a vacuum in GEANT4, with the desired goal of losing most of the 220Rn (and thus the hard gamma from 208Tl and the residual 208Pb mass). GEANT4 handles the particle physics, but I obviously have to model the diffusion myself. 220Rn has a half life of 55,6s, while modeled diffusion times through the pores are typically on the order of a few hundred milliseconds, so no issues there.
The issue becomes the time for diffusion from the matrix into the pore space. With varying assumptions, in an unmodified bulk solid, I get solid diffusion times on the order of a couple minutes to an hour or more - too long, but tantalizingly close when dealing with systems where variations in rates tend to be on order-of-magnitude scales. And there is a serious complication: the damage to the matrix from the deceleration of the recoiling 220Rn (~100keV).
1) My understanding from research in bulk solids is that preexisting tracks in crystalline oxides tend to be immobilizing to diffusion, but for a very brief period, the track is a hot, chaotic mess before it cools and the bond structure stabilizes. I don't expect the daughters to go far during this (incredibly brief) period, but then again, they don't have far to go.
2) When dealing with aerogels, we're dealing with an incredibly fine, delicate structure to begin with, which raises the question of localized diffusion enhancement mechanisms, such as microcracking (indeed, there's a question of microcracks to begin with...), voids, etc. Also, UO3 is chemically disfavored at elevated temperatures (will lose oxygen at 750°C even in pure O2 at 5ATM), so there's the possibility of UO2 or U3O8 formation with free oxygen and grain boundaries.
Any idea how I could reasonably model this, or am I basically SOL without experimental data? My attempts to dig up preexisting research haven't proved fruitful.
(Precision isn't needed, but order-of-magnitude is. In all likelihood, it's "nearly all diffuses into the pore space" or "nearly none diffuses into the pore space")
The issue becomes the time for diffusion from the matrix into the pore space. With varying assumptions, in an unmodified bulk solid, I get solid diffusion times on the order of a couple minutes to an hour or more - too long, but tantalizingly close when dealing with systems where variations in rates tend to be on order-of-magnitude scales. And there is a serious complication: the damage to the matrix from the deceleration of the recoiling 220Rn (~100keV).
1) My understanding from research in bulk solids is that preexisting tracks in crystalline oxides tend to be immobilizing to diffusion, but for a very brief period, the track is a hot, chaotic mess before it cools and the bond structure stabilizes. I don't expect the daughters to go far during this (incredibly brief) period, but then again, they don't have far to go.
2) When dealing with aerogels, we're dealing with an incredibly fine, delicate structure to begin with, which raises the question of localized diffusion enhancement mechanisms, such as microcracking (indeed, there's a question of microcracks to begin with...), voids, etc. Also, UO3 is chemically disfavored at elevated temperatures (will lose oxygen at 750°C even in pure O2 at 5ATM), so there's the possibility of UO2 or U3O8 formation with free oxygen and grain boundaries.
Any idea how I could reasonably model this, or am I basically SOL without experimental data? My attempts to dig up preexisting research haven't proved fruitful.
(Precision isn't needed, but order-of-magnitude is. In all likelihood, it's "nearly all diffuses into the pore space" or "nearly none diffuses into the pore space")
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