Radiation-Induced Interfacial Hydroxyl Transformation on Boehmite and Gibbsite Basal Surfaces

Sassi, Michel; Walter, Eric D.; Qafoku, Odeta; Rosso, Kevin M.; Wang, Zheming

doi:10.1021/acs.jpcc.0c06844

Radiation-Induced Interfacial Hydroxyl Transformation on Boehmite and Gibbsite Basal Surfaces

Journal Article · Fri Sep 11 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c06844· OSTI ID:1721691

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Understanding the radiolytic reactivity of aluminum oxyhydroxide phases widely present in stored nuclear wastes is essential to develop reliable processing approaches. Recent experiments using vibrational sum frequency generation (VSFG), a surface sensitive technique, have shown that rehydration of γ-irradiated boehmite (010) and gibbsite (001) surfaces does not recover the initial hydroxyl density prior to irradiation. In this study, using density functional theory and nudged elastic band calculations, we examine dehydration and rehydration of these surfaces and attendant proton transfer mechanisms. While dehydration of both surfaces is predicted to be energetically unfavorable, rehydration of boehmite (010) is favorable after overcoming an energy barrier of 0.52 eV that relates to the orientation of surface hydroxyls controlling the hydrogen bonding network of adsorbed water. In the case of gibbsite (001), for which the experimental results suggest that rehydration mainly involves the reformation of interlayer hydroxyls, we found that a two-proton transfer mechanism is more likely than a one-proton transfer mechanism, and that it prevents the reorientation of interlayer hydroxyls into intralayer hydroxyls consistent with experimental VSFG findings. A detailed analysis of the effect of surface hydrogen vacancy on the strength of hydrogen bond interactions was performed, which indicates that H₂ and H₂O are the energetically most favorable product species to form from radiation-induced surface H and/or OH defects.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1721691

Report Number(s):: PNNL-SA-153541

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 40 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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