Phase separation of stable colloidal clusters
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PhysRevMaterials.2.095602.pdf
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Author(s) • • •
Petersen, Thomas
Bazant, Martin Z
Pellenq, Roland Jm
Ulm, Franz-Josef
Date Issued
September 2018
Journal
Physical Review Materials
Publisher
American Physical Society
Citation
Petersen, Thomas et al. "Phase separation of stable colloidal clusters." Physical Review Materials 2, 9 (September 2018): 095602 © 2018 American Physical Society
Version
Final published version
Abstract
This article presents a nonequilibrium thermodynamic theory for the mean-field precipitation, aggregation, and pattern formation of colloidal clusters. A variable gradient energy coefficient and the arrest of particle diffusion upon “jamming” of cluster aggregates in the spinodal region predicts observable gel patterns that, at high intercluster attraction, form system-spanning, out-of-equilibrium networks with glasslike, quasistatic structural relaxation. For reactive systems, we incorporate the free energy landscape of stable prenucleation clusters into the Allen-Cahn reaction equation. We show that pattern formation is dominantly controlled by the Damköhler number and the stability of the clusters, which modifies the autocatalytic rate of precipitation. As clusters individually become more stable, bulk phase separation is suppressed.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
Massachusetts Institute of Technology. Department of Mathematics
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DOI of Published Version
https://doi.org/10.1103/PhysRevMaterials.2.095602