Radiolysis and Radiation-Driven Dynamics of Boehmite Dissolution Observed by in Situ Liquid-Phase TEM

Lili Liu, Jaehun Chun, Xin Zhang, Michel Sassi, Andrew G. Stack, Carolyn I. Pearce, Sue B. Clark, Kevin M. Rosso, James J. De Yoreo, Greg A. Kimmel

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

Over the last several decades, there have been several studies examining the radiation stability of boehmite and other aluminum oxyhydroxides, yet less is known about the impact of radiation on boehmite dissolution. Here, we investigate radiation effects on the dissolution behavior of boehmite by employing liquid-phase transmission electron microscopy (LPTEM) and varying the electron flux on the samples consisting of either single nanoplatelets or aggregated stacks. We show that boehmite nanoplatelets projected along the [010] direction exhibit uniform dissolution with a strong dependence on the electron dose rate. For nanoplatelets that have undergone oriented aggregation, we show that the dissolution occurs preferentially at the particles at the ends of the stacks that are more accessible to bulk solution than at the others inside the aggregate. In addition, at higher dose rates, electrostatic repulsion and knock-on damage from the electron beam causes delamination of the stacks and dissolution at the interfaces between particles in the aggregate, indicating that there is a threshold dose rate for electron-beam enhancement of dissolution of boehmite aggregates.

Original languageEnglish
Pages (from-to)5029-5036
Number of pages8
JournalEnvironmental Science and Technology
Volume56
Issue number8
DOIs
StatePublished - Apr 19 2022

Funding

This work was fully supported by IDREAM (Interfacial Dynamics in Radioactive Environments and Materials), an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences. All Liquid cell TEM experiments were performed in the Environmental and Molecular Sciences Laboratory, which is an Office of Biological and Environmental Research user facility located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract No. DEAC05-76RLO1830.

FundersFunder number
IDREAM
U.S. Department of EnergyDEAC05-76RLO1830
Office of Science
Basic Energy Sciences

    Keywords

    • aggregation
    • boehmite
    • dissolution
    • liquid-phase TEM

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