Determining Radiolytic Transient Intermediates and Interfacial Species and Their Roles in Aluminum Oxyhydroxide Reactivity
EMSL Project ID
50151
Abstract
Radiation-induced chemical reactions have broad significance in many scientific fields from water radiolysis in nuclear reactors and nuclear fuel design to spent nuclear fuel storage and high-level nuclear waste reprocessing. Multiple lines of evidence have suggested that interfacial chemistry and energy transfer processes at the interfaces play important roles in radiation induced chemical transformations in heterogeneous systems. However, as post-irradiation chemical reactions mostly occur on the time scales of femto-second to microsecond time scale, deterministic studies of the radiation-induced reactions are hindered by the short process lifetimes and low concentrations of the reactive transient intermediates due to lack of proper ultrafast techniques, particularly those that target speciation and energy transfer processes at solid-liquid interfaces. In this project, we develop and apply a suite of in situ electron paramagnetic resonance spectroscopy techniques to identify and quantify the radiolytic transient species and their temporal evolution profiles, to reveal the interfacial hydration and hydroxylation structure and energetic behavior, and unravel their roles in aluminum oxyhydroxide transformation processes under irradiated conditions. In the later stage of the project, research will also be applied to investigate the interfacial chemistry of zirconium oxide and its effect on water radiolysis. The selected chemical systems, while representing typical dielectric metal oxyhydroxides from a fundamental chemistry point of view, are widely used in the nuclear industry as cladding and casing materials and thus our research is expected to offer insights into spent nuclear fuel processing, high-level waste handling and storage as well as potential nuclear forensic applications.
Project Details
Start Date
2018-01-30
End Date
2020-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Walter E.D., K.C. Schwarz, S. Anil Kumar, Y. Chen, M. Sassi, Z. Wang, and K.M. Rosso. 2020. "Evolution of Radicals from the Photolysis of High Ionic Strength Alkaline Nitrite Solutions." Journal of Physical Chemistry A 124, no. 16:3019-3025. PNNL-SA-150363. doi:10.1021/acs.jpca.9b11438