Crystal dissolution by particle detachment
Abstract
Crystal dissolution, which is a fundamental process in both natural and technological settings, has been predominately viewed as a process of ion-by-ion detachment into a surrounding solvent. Here we report a mechanism of dissolution by particle detachment (DPD) that dominates in mesocrystals formed via crystallization by particle attachment (CPA). Using liquid phase electron microscopy to directly observe dissolution of hematite crystals — both compact rhombohedra and mesocrystals of coaligned nanoparticles — we find that the mesocrystals evolve into branched structures, which disintegrate as individual sub-particles detach. The resulting dissolution rates far exceed those for equivalent masses of compact single crystals. Applying a numerical generalization of the Gibbs-Thomson effect, we show that the physical drivers of DPD are curvature and strain inherently tied to the original CPA process. Based on the generality of the model, we anticipate that DPD is widespread for both natural minerals and synthetic crystals formed via CPA.
- Authors:
-
[1];
[2];
[1]
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); University of Washington, Seattle, WA (United States)
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 2300540
- Report Number(s):
- PNNL-SA-190350
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- AC05-76RL01830; 56674
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; material science; techniques and instrumentation
Citation Formats
Zhu, Guomin, Legg, Benjamin A., Sassi, Michel, Liang, Xinran, Zong, Meirong, Rosso, Kevin M., and De Yoreo, James J. Crystal dissolution by particle detachment. United States: N. p., 2023.
Web. doi:10.1038/s41467-023-41443-y.
Zhu, Guomin, Legg, Benjamin A., Sassi, Michel, Liang, Xinran, Zong, Meirong, Rosso, Kevin M., & De Yoreo, James J. Crystal dissolution by particle detachment. United States. https://doi.org/10.1038/s41467-023-41443-y
Zhu, Guomin, Legg, Benjamin A., Sassi, Michel, Liang, Xinran, Zong, Meirong, Rosso, Kevin M., and De Yoreo, James J. Mon .
"Crystal dissolution by particle detachment". United States. https://doi.org/10.1038/s41467-023-41443-y. https://www.osti.gov/servlets/purl/2300540.
@article{osti_2300540,
title = {Crystal dissolution by particle detachment},
author = {Zhu, Guomin and Legg, Benjamin A. and Sassi, Michel and Liang, Xinran and Zong, Meirong and Rosso, Kevin M. and De Yoreo, James J.},
abstractNote = {Crystal dissolution, which is a fundamental process in both natural and technological settings, has been predominately viewed as a process of ion-by-ion detachment into a surrounding solvent. Here we report a mechanism of dissolution by particle detachment (DPD) that dominates in mesocrystals formed via crystallization by particle attachment (CPA). Using liquid phase electron microscopy to directly observe dissolution of hematite crystals — both compact rhombohedra and mesocrystals of coaligned nanoparticles — we find that the mesocrystals evolve into branched structures, which disintegrate as individual sub-particles detach. The resulting dissolution rates far exceed those for equivalent masses of compact single crystals. Applying a numerical generalization of the Gibbs-Thomson effect, we show that the physical drivers of DPD are curvature and strain inherently tied to the original CPA process. Based on the generality of the model, we anticipate that DPD is widespread for both natural minerals and synthetic crystals formed via CPA.},
doi = {10.1038/s41467-023-41443-y},
journal = {Nature Communications},
number = 1,
volume = 14,
place = {United States},
year = {Mon Oct 09 00:00:00 EDT 2023},
month = {Mon Oct 09 00:00:00 EDT 2023}
}
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