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Title: Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution

Abstract

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 thermodynamicsmore » of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.« less

Authors:
 [1];  [2];  [3];  [4];  [5]
  1. Clemson Univ., SC (United States)
  2. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
  3. Univ. of Illinois, Urbana-Champaign, IL (United States)
  4. Univ. of Michigan, Ann Arbor, MI (United States)
  5. Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Clemson Univ., SC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1367657
Report Number(s):
RPT-0000001045
DOE Contract Number:  
SC0004883
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; actinide; plutonium; lysimeter; radiochemistry; sorption; surface complexation model

Citation Formats

Powell, Brian, Kaplan, Daniel I, Arai, Yuji, Becker, Udo, and Ewing, Rod. Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution. United States: N. p., 2016. Web. doi:10.2172/1367657.
Powell, Brian, Kaplan, Daniel I, Arai, Yuji, Becker, Udo, & Ewing, Rod. Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution. United States. https://doi.org/10.2172/1367657
Powell, Brian, Kaplan, Daniel I, Arai, Yuji, Becker, Udo, and Ewing, Rod. 2016. "Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution". United States. https://doi.org/10.2172/1367657. https://www.osti.gov/servlets/purl/1367657.
@article{osti_1367657,
title = {Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution},
author = {Powell, Brian and Kaplan, Daniel I and Arai, Yuji and Becker, Udo and Ewing, Rod},
abstractNote = {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.},
doi = {10.2172/1367657},
url = {https://www.osti.gov/biblio/1367657}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Dec 29 00:00:00 EST 2016},
month = {Thu Dec 29 00:00:00 EST 2016}
}