Effect of Background Electrolyte Composition on the Interfacial Formation of Th(IV) Nanoparticles on the Muscovite (001) Basal Plane

Neumann, J; Qiu, C; Eng, P; Skanthakumar, S.; Soderholm, L.; Stumpf, T; Schmidt, M

doi:10.1021/acs.jpcc.1c03997

Effect of Background Electrolyte Composition on the Interfacial Formation of Th(IV) Nanoparticles on the Muscovite (001) Basal Plane

Journal Article · 05 August 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c03997· OSTI ID:1838931

Neumann, J; Qiu, C; Eng, P; Skanthakumar, S.; Soderholm, L.; Stumpf, T; Schmidt, M

Understanding the impact of actinide nanoparticle (NP) formation is important to assess radionuclide mobility in the environment. We combined surface X-ray diffraction (SXRD) and in situ AFM to investigate the previously reported unusual electrolyte effects on Th uptake on mica. At low [Th] (0.1 mM), interfacial structures show a broad Th electron density (~50 Å). A linear decrease of Th uptake with decreasing hydration enthalpy of the electrolyte cation (Li+, K+, NH4+, and Cs+) indicates a competitive effect between Th and the electrolyte cation. Na+ is a clear outlier from this trend. In situ AFM imaging confirms the results. Particles show a vertical size of ~1–2 nm and larger lateral dimensions of ~10–20 nm, which is typical for particles formed at interfaces (heterogeneous nucleation). At high [Th] = 1 and 3 mM, all investigated electrolytes (ACl, A = Li+, Na+, K+) show similar Th uptake, indicating a much smaller impact of electrolyte composition. The interfacial structures are dominated by a high Th loading at a distinct distance (~6.5 Å) from the surface. Therefore, the main retention mechanism at high [Th] is suggested to be the sorption of Th NPs aggregated from Th oligomers present in solution (homogeneous nucleation).

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division; National Science Foundation (NSF) - Directorate for Geosciences Division of Earth Sciences (GEO/EAR)

DOE Contract Number:: AC02-06CH11357

OSTI ID:: 1838931

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 30

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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