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@ARTICLE{Deng:911141,
author = {Deng, Hang and Poonoosamy, Jenna and Molins, Sergi},
title = {{A} reactive transport modeling perspective on the dynamics
of interface-coupled dissolution-precipitation},
journal = {Applied geochemistry},
volume = {137},
issn = {0883-2927},
address = {Amsterdam [u.a.]},
publisher = {Elsevier Science},
reportid = {FZJ-2022-04457},
pages = {105207 -},
year = {2022},
abstract = {In interface coupled dissolution-precipitation systems, the
dynamics of the mineral-fluid interface depends on two
intertwining processes: the dissolution of the primary
mineral that is needed for subsequent precipitation and the
passivation of the dissolution reaction as a result of
secondary mineral precipitation. The resulting thickness and
texture of the precipitating coating layer will affect the
progression of geochemical reactions, flow and transport
processes at the macroscopic scale. Understanding the
interplay between macroscopic flow regimes and microscopic
reaction mechanisms (e.g., nucleation and crystal growth
pathways) in controlling the dynamics of the mineral-fluid
interface has important implications for predicting natural
weathering processes, scaling in the subsurface energy
production systems, etc. In this study, we use a
micro-continuum pore-scale reactive transport model to
investigate the feedback loop between reaction rate and
solute transport with explicit consideration of the surface
passivation and the diffusion process through the coating
layer, as well as the impacts of saturation-dependent
nucleation rate on the textures of precipitates that will
largely dictate the diffusion properties of the coating
layer. Our model results highlight that the drastically
different coating behaviors at the macroscopic scale and
their dependence on solution supersaturation observed in
previous column experiments are primarily controlled by the
interplay between mineral reaction rates, advective flow,
and diffusion through the dynamically forming coating layer.
The diffusion properties of the coating layer also play a
secondary but non-negligible role in shaping the evolution
of the co-dissolution and precipitation system. The
probabilistic nucleation model building on the framework of
classical nucleation theory highlights the complex
dependence of precipitates’ texture on solution chemistry
and substrate properties, which can affect the diffusion
process within the precipitates. The modeling observations
also underscore the necessity of further investigations to
better characterize the properties of the coating layer and
to improve modeling descriptions of the nucleation
processes.},
cin = {IEK-6},
ddc = {550},
cid = {I:(DE-Juel1)IEK-6-20101013},
pnm = {1411 - Nuclear Waste Disposal (POF4-141)},
pid = {G:(DE-HGF)POF4-1411},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000798069300006},
doi = {10.1016/j.apgeochem.2022.105207},
url = {https://juser.fz-juelich.de/record/911141},
}