Abstract
Spent nuclear fuel contains both uranium (U) and high yield fission products, including strontium-90 ((90)Sr), a key radioactive contaminant at nuclear facilities. Both U and (90)Sr will be present where spent nuclear fuel has been processed, including in storage ponds and tanks. However, the interactions between Sr and U phases under ambient conditions are not well understood. Over a pH range of 4-14, we investigate Sr sorption behavior in contact with two nuclear fuel cycle relevant U(IV) phases: nano-uraninite (UO(2)) and U(IV)-silicate nanoparticles. Nano-UO(2) is a product of the anaerobic corrosion of metallic uranium fuel, and UO(2) is also the predominant form of U in ceramic fuels. U(IV)-silicates form stable colloids under the neutral to alkaline pH conditions highly relevant to nuclear fuel storage ponds and geodisposal scenarios. In sorption experiments, Sr had the highest affinity for UO(2), although significant Sr sorption also occurred to U(IV)-silicate phases at pH ≥ 6. Extended X-ray absorption fine structure (EXAFS) spectroscopy, transmission electron microscopy, and desorption data for the UO(2) system suggested that Sr interacted with UO(2) via a near surface, highly coordinated complex at pH ≥ 10. EXAFS measurements for the U(IV)-silicate samples showed outer-sphere Sr sorption dominated at acidic and near-neutral pH with intrinsic Sr-silicates forming at pH ≥ 12. These complex interactions of Sr with important U(IV) phases highlight a largely unrecognized control on (90)Sr mobility in environments of relevance to spent nuclear fuel management and storage.