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.