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Title: Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site

Abstract

This paper reviews the origin and chemical and rheological complexity of radioactive waste at the U.S. Department of Energy’s Hanford Site. The waste, stored in underground tanks, was generated via three distinct processes over decades of plutonium extraction operations. Although close records were kept of original waste disposition, tank-to-tank transfers and conditions that impede equilibrium complicate our understanding of the chemistry, phase composition, and rheology of the waste. Tank waste slurries comprise particles and aggregates from nano to micron scales, with varying densities, morphologies, heterogeneous compositions, and complicated responses to flow regimes and process conditions. Further, remnant or changing radiation fields may affect the stability and rheology of the waste. These conditions pose challenges for transport through conduits or pipes to treatment plants for vitrification. Additionally, recalcitrant boehmite degrades glass quality and must be reduced prior to vitrification, but dissolves much more slowly than predicted given surface normalized rates. Existing empirical models based on ex situ experiments and observations lack true predictive capabilities. Recent advances in in situ microscopy, aberration corrected TEM, theoretical modeling across scales, and experimental methods for probing the physics and chemistry at mineral-fluid and mineral-mineral interfaces are being implemented to build robustly predictive physics-based models.

Authors:
; ; ; ;  [1]; ORCiD logo; ORCiD logo;  [2]
  1. Washington River Protection Solutions, Richland, Washington 99354, United States
  2. Chemistry Department, Washington State University, Pullman, Washington 99164, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1422287
Report Number(s):
PNNL-SA-128559
Journal ID: ISSN 0013-936X; 49654
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Environmental Science and Technology; Journal Volume: 52; Journal Issue: 2
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Peterson, Reid A., Buck, Edgar C., Chun, Jaehun, Daniel, Richard C., Herting, Daniel L., Ilton, Eugene S., Lumetta, Gregg J., and Clark, Sue B. Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site. United States: N. p., 2018. Web. doi:10.1021/acs.est.7b04077.
Peterson, Reid A., Buck, Edgar C., Chun, Jaehun, Daniel, Richard C., Herting, Daniel L., Ilton, Eugene S., Lumetta, Gregg J., & Clark, Sue B. Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site. United States. doi:10.1021/acs.est.7b04077.
Peterson, Reid A., Buck, Edgar C., Chun, Jaehun, Daniel, Richard C., Herting, Daniel L., Ilton, Eugene S., Lumetta, Gregg J., and Clark, Sue B. Tue . "Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site". United States. doi:10.1021/acs.est.7b04077.
@article{osti_1422287,
title = {Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site},
author = {Peterson, Reid A. and Buck, Edgar C. and Chun, Jaehun and Daniel, Richard C. and Herting, Daniel L. and Ilton, Eugene S. and Lumetta, Gregg J. and Clark, Sue B.},
abstractNote = {This paper reviews the origin and chemical and rheological complexity of radioactive waste at the U.S. Department of Energy’s Hanford Site. The waste, stored in underground tanks, was generated via three distinct processes over decades of plutonium extraction operations. Although close records were kept of original waste disposition, tank-to-tank transfers and conditions that impede equilibrium complicate our understanding of the chemistry, phase composition, and rheology of the waste. Tank waste slurries comprise particles and aggregates from nano to micron scales, with varying densities, morphologies, heterogeneous compositions, and complicated responses to flow regimes and process conditions. Further, remnant or changing radiation fields may affect the stability and rheology of the waste. These conditions pose challenges for transport through conduits or pipes to treatment plants for vitrification. Additionally, recalcitrant boehmite degrades glass quality and must be reduced prior to vitrification, but dissolves much more slowly than predicted given surface normalized rates. Existing empirical models based on ex situ experiments and observations lack true predictive capabilities. Recent advances in in situ microscopy, aberration corrected TEM, theoretical modeling across scales, and experimental methods for probing the physics and chemistry at mineral-fluid and mineral-mineral interfaces are being implemented to build robustly predictive physics-based models.},
doi = {10.1021/acs.est.7b04077},
journal = {Environmental Science and Technology},
number = 2,
volume = 52,
place = {United States},
year = {Tue Jan 02 00:00:00 EST 2018},
month = {Tue Jan 02 00:00:00 EST 2018}
}