Crystal dissolution by particle detachment

Guomin Zhu, Benjamin A. Legg, Michel Sassi, Xinran Liang, Meirong Zong, Kevin M. Rosso and James J. Yoreo ()
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Guomin Zhu: Pacific Northwest National Laboratory
Benjamin A. Legg: Pacific Northwest National Laboratory
Michel Sassi: Pacific Northwest National Laboratory
Xinran Liang: Pacific Northwest National Laboratory
Meirong Zong: Pacific Northwest National Laboratory
Kevin M. Rosso: Pacific Northwest National Laboratory
James J. Yoreo: Pacific Northwest National Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-41443-y

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