Silicon Control of Strontium and Cesium Partitioning in Hydroxide-Weathered Sediments

Journal Article · Tue Apr 15 04:00:00 EDT 2008 · Geochimica et Cosmochimica Acta, 72(8):2024-2047

DOI:https://doi.org/10.1016/j.gca.2008.01.026· OSTI ID:934625

Chorover, Jon; Choi, Sunkyung; Rotenberg, P; Serne, R Jeffrey; Rivera, Nelson; Strepka, Caleb R; Thompson, Aaron; Mueller, Karl T; O'Day, Peggy A

Cation partitioning in an aqueous soil suspension depends on the coupling of reaction time, sorbate amount and mineral weathering reactions. These factors were varied in sediment suspension experiments to identify geochemical processes that affect migration of Sr2+ and Cs+ introduced to the subsurface by caustic high level radioactive waste (HLRW). Three glacio-fluvial and lacustrine sediments from the Hanford Site were subjected to hyperalkaline (pH > 13), Na–Al–NO3–OH solution conditions within a gradient field of (i) sorptive concentration (10-5–10-3 M) and (ii) reaction time (0–365 d). Strontium uptake (qSr) exceeded that of cesium at nearly all reaction times. Sorbent affinity for both Cs+ and Sr2+ increased with clay plus silt content at early times, but a prolonged slow uptake process was observed over the course of sediment weathering that erased the texture effect for Sr2+; all sediments showed similar mass normalized uptake after several months of reaction time. Strontium became progressively recalcitrant to desorption after 92 d, with accumulation and aging of neoformed aluminosilicates. Formation of Cs+ and Sr2+-containing cancrinite and sodalite was observed after 183 d by SEM and synchrotron u-XRF and u-XRD. EXAFS data showed ncorporation of Sr2+ into both feldspathoid and SrCO3(s) coordination environments after one year. Adsorption was predominant at early times and low sorbate amount, whereas recipitation, controlled largely by sediment Si release, became increasingly important at longer times and higher sorbate amount. Kinetics of contaminant desorption at pH 8 from one year-weathered sediments showed significant dependence on background cation (Ca2+ versus K+) composition. Results of this study indicate that co-precipitation and ion exchange in neoformed aluminosilicates may be an important mechanism controlling Sr2+ and Cs+ mobility in siliceous sediments impacted by hyperalkaline HLRW.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 934625
• Report Number(s): PNNL-SA-60417; 10292; 21595; 3101; KP1302000
• Journal Information: Geochimica et Cosmochimica Acta, 72(8):2024-2047, Journal Name: Geochimica et Cosmochimica Acta, 72(8):2024-2047 Journal Issue: 8 Vol. 72; ISSN GCACAK; ISSN 0016-7037
• Country of Publication: United States
• Language: English

Related Subjects

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
43 PARTICLE ACCELERATORS
ADSORPTION
AFFINITY
AGING
CATIONS
CESIUM
CLAYS
DESORPTION
Environmental Molecular Sciences Laboratory
ION EXCHANGE
KINETICS
RADIOACTIVE WASTES
SEDIMENTS
SILICON
SILT
SOILS
STRONTIUM
SYNCHROTRONS
TEXTURE
WEATHERING
high-level tank waste
sorption of Sr and Cs
tank waste-sediment interactions