4.8 Article

Radiolysis and Radiation-Driven Dynamics of Boehmite DissolutionObserved by In Situ Liquid-Phase TEM

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 8, Pages 5029-5036

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c08415

Keywords

boehmite; dissolution; aggregation; liquid-phase TEM

Funding

  1. IDREAM (Interfacial Dynamics in Radioactive Environments and Materials), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences
  2. Department of Energy [DEAC05-76RLO1830]

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This study investigates the radiation effects on the dissolution behavior of boehmite using liquid-phase transmission electron microscopy. The results show that the dissolution of boehmite varies with different electron dose rates, and electrostatic repulsion and knock-on damage from the electron beam can enhance the dissolution process.
Over the last several decades, there have been several studies examiningthe radiation stability of boehmite and other aluminum oxyhydroxides, yet less isknown about the impact of radiation on boehmite dissolution. Here, we investigateradiation effects on the dissolution behavior of boehmite by employing liquid-phasetransmission electron microscopy (LPTEM) and varying the electronflux on thesamples consisting of either single nanoplatelets or aggregated stacks. We show thatboehmite nanoplatelets projected along the [010] direction exhibit uniform dissolutionwith a strong dependence on the electron dose rate. For nanoplatelets that haveundergone oriented aggregation, we show that the dissolution occurs preferentially atthe particles at the ends of the stacks that are more accessible to bulk solution than atthe others inside the aggregate. In addition, at higher dose rates, electrostatic repulsionand knock-on damage from the electron beam causes delamination of the stacks anddissolution at the interfaces between particles in the aggregate, indicating that there is athreshold dose rate for electron-beam enhancement of dissolution of boehmite aggregates

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