Long-term Kinetics of Uranyl Desorption from Sediments Under Advective Conditions

Journal Article · Sat Feb 15 04:00:00 EST 2014 · Water Resources Research, 50(2):855-870

DOI:https://doi.org/10.1002/2013WR013949· OSTI ID:1136607

Shang, Jianying; Liu, Chongxuan; Wang, Zheming; Zachara, John M.

Long-term (> 4 months) column experiments were performed to investigate the kinetics of uranyl (U(VI)) desorption in sediments collected from the Integrated Field Research Challenge (IFRC) site at the US Department of Energy (DOE) Hanford 300 Area. The experimental results were used to evaluate alternative multi-rate surface complexation reaction (SCR) approaches to describe the short- and long-term kinetics of U(VI) desorption under flow conditions. The SCR stoichiometry, equilibrium constants, and multi-rate parameters were independently characterized in batch and stirred flow-cell reactors. Multi-rate SCR models that were either additively constructed using the SCRs for individual size fractions (e.g., Shang et al., 2011), or composite in nature could effectively describe short-term U(VI) desorption under flow conditions. The long-term desorption results, however, revealed that using a labile U concentration measured by carbonate extraction under-estimated desorbable U(VI) and the long-term rate of U(VI) desorption. An alternative modeling approach using total U as the desorbable U(VI) concentration was proposed to overcome this difficulty. This study also found that the gravel size fraction (2-8 mm), which is typically treated as non-reactive in modeling U(VI) reactive transport because of low external surface area, can have an important effect on the U(VI) desorption in the sediment. This study demonstrates an approach to effectively extrapolate U(VI) desorption kinetics for field-scale application, and identifies important parameters and uncertainties affecting model predictions.

• 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: 1136607
• Report Number(s): PNNL-SA-94505; 47712; KP1702030
• Journal Information: Water Resources Research, 50(2):855-870, Journal Name: Water Resources Research, 50(2):855-870
• Country of Publication: United States
• Language: English

Related Subjects

Environmental Molecular Sciences Laboratory
Kinetics
Long-term
Uranyl Desorption
additivity approach
heterogeneous