Unraveling pH-Dependent Changes in Adsorption Structure of Uranyl on Alumina (012)

Neumann, Julia; Carr, Amanda J.; Lessing, Jessica; Soderholm, L.; Catalano, Jeffrey G.; Fenter, Paul; Lee, Sang Soo

doi:10.1021/acs.jpclett.4c00498

Unraveling pH-Dependent Changes in Adsorption Structure of Uranyl on Alumina (012)

Journal Article · Fri Mar 22 00:00:00 EDT 2024 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.4c00498· OSTI ID:2497710

^[1]; ^[1]; Lessing, Jessica ^[2]; ^[1]; ^[3]; ^[1]; ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Helmholtz-Zentrum Dresden-Rossendorf, (Germany). Institute of Resource Ecology
Washington Univ., St. Louis, MO (United States)

Mitigating uranium transport in groundwater is imperative for ensuring access to clean water across the globe. Here, in situ resonant anomalous X-ray reflectivity is used to investigate the adsorption of uranyl on alumina (012) in acidic aqueous solutions, representing typical U^VI concentrations of contaminated water near mining sites. The analyses reveal that U^VI adsorbs at two distinct heights of 2.4-3.2 and 5-5.3 angstrom from the surface terminal oxygens. The former is interpreted as the mixture of inner-sphere and outer-sphere complexes that adsorb closest to the surface. The latter is interpreted as an outer-sphere complex that shares one equatorial H₂O with the terminal surface oxygen. With increasing pH, we observe an increasing prevalence of these outer-sphere complexes, indicating the enhanced role of the hydrogen bond that stabilizes adsorbed uranyl species. Finally, the presented work provides a molecular-scale understanding of sorption of uranyl on Al-based-oxide surfaces that has implications for environmental chemistry and materials science.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: German Federal Ministry for the Environment, Nature Conservation, Nuclear Safety, and Consumer Protection; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357; SC0022213

OSTI ID:: 2497710

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 13 Vol. 15; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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