Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution
- Clemson Univ., SC (United States)
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Univ. of Illinois, Urbana-Champaign, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Stanford Univ., CA (United States)
This university lead SBR project is a collaboration lead by Dr. Brian Powell (Clemson University) with co-principal investigators Dan Kaplan (Savannah River National Laboratory), Yuji Arai (presently at the University of Illinois), Udo Becker (U of Michigan) and Rod Ewing (presently at Stanford University). Hypothesis: The underlying hypothesis of this work is that strong interactions of plutonium with mineral surfaces are due to formation of inner sphere complexes with a limited number of high-energy surface sites, which results in sorption hysteresis where Pu(IV) is the predominant sorbed oxidation state. The energetic favorability of the Pu(IV) surface complex is strongly influenced by positive sorption entropies, which are mechanistically driven by displacement of solvating water molecules from the actinide and mineral surface during sorption. Objectives: The overarching objective of this work is to examine Pu(IV) and Pu(V) sorption to pure metal (oxyhydr)oxide minerals and sediments using variable temperature batch sorption, X-ray absorption spectroscopy, electron microscopy, and quantum-mechanical and empirical-potential calculations. The data will be compiled into a self-consistent surface complexation model. The novelty of this effort lies largely in the manner the information from these measurements and calculations will be combined into a model that will be used to evaluate the thermodynamics of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.
- Research Organization:
- Clemson Univ., SC (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- DOE Contract Number:
- SC0004883
- OSTI ID:
- 1367657
- Report Number(s):
- RPT-0000001045
- Country of Publication:
- United States
- Language:
- English
Similar Records
Quantification of Cation Sorption to Engineered Barrier Materials Under Extreme Conditions
Plutonium environmental chemistry: mechanisms for the surface-mediated reduction of Pu(v/vi)