Crystal dissolution by particle detachment

Zhu, Guomin; Legg, Benjamin A.; Sassi, Michel; Liang, Xinran; Zong, Meirong; Rosso, Kevin M.; De Yoreo, James J.

doi:10.1038/s41467-023-41443-y

Title: Crystal dissolution by particle detachment

Journal Article · 08 October 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-41443-y · OSTI ID:2300540

^[1]; Legg, Benjamin A. ^[2]; Sassi, Michel ^[2]; Liang, Xinran ^[2]; Zong, Meirong ^[2];

^[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)

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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: 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)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2300540

Report Number(s):: PNNL-SA--190350

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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