skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Processing High Level Waste: Spectroscopic Characterization of Redox Reactions in Supercritical Water

Abstract

We are engaged in a collaborative research effort with Los Alamos staff scientists Steven Buelow and Jeanne Robinson, staff members in group CST-6. The work proposed by these LANL staff scientists is directed towards the destruction of complexants and oxidation of chromium and technetium by hydrothermal processing in near critical or supercritical aqueous solutions. Our own work has been focused on a careful kinetic study of oxidation reactions of hydrogen peroxide with chromium hydroxide. This reaction occurs readily at ambient temperatures.

Authors:
Publication Date:
Research Org.:
Furman University, Greenville, SC (US)
Sponsoring Org.:
USDOE Office of Environmental Management (EM) (US)
OSTI Identifier:
827200
Report Number(s):
EMSP-54828-2000
R&D Project: EMSP 54828; TRN: US200425%%469
DOE Contract Number:
FG07-96ER14709
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: 1 Jun 2000
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; 54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; AMBIENT TEMPERATURE; AQUEOUS SOLUTIONS; CHROMIUM; CHROMIUM HYDROXIDES; HYDROGEN PEROXIDE; KINETICS; OXIDATION; PROCESSING; REDOX REACTIONS; TECHNETIUM; WATER

Citation Formats

Arrington, Jr., Charles A.. Processing High Level Waste: Spectroscopic Characterization of Redox Reactions in Supercritical Water. United States: N. p., 2000. Web. doi:10.2172/827200.
Arrington, Jr., Charles A.. Processing High Level Waste: Spectroscopic Characterization of Redox Reactions in Supercritical Water. United States. doi:10.2172/827200.
Arrington, Jr., Charles A.. Thu . "Processing High Level Waste: Spectroscopic Characterization of Redox Reactions in Supercritical Water". United States. doi:10.2172/827200. https://www.osti.gov/servlets/purl/827200.
@article{osti_827200,
title = {Processing High Level Waste: Spectroscopic Characterization of Redox Reactions in Supercritical Water},
author = {Arrington, Jr., Charles A.},
abstractNote = {We are engaged in a collaborative research effort with Los Alamos staff scientists Steven Buelow and Jeanne Robinson, staff members in group CST-6. The work proposed by these LANL staff scientists is directed towards the destruction of complexants and oxidation of chromium and technetium by hydrothermal processing in near critical or supercritical aqueous solutions. Our own work has been focused on a careful kinetic study of oxidation reactions of hydrogen peroxide with chromium hydroxide. This reaction occurs readily at ambient temperatures.},
doi = {10.2172/827200},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Jun 01 00:00:00 EDT 2000},
month = {Thu Jun 01 00:00:00 EDT 2000}
}

Technical Report:

Save / Share:
  • 'All of the work done so far was carried out at Los Alamos National Lab. During the summer program at LANL all equipment and supplies were provided through Dr. Buelow''s program at LANL. The author is now setting up a Raman spectroscopy lab at Furman. Using departmental funds he has purchased an optical bench, a laser, and a CCD detector and are ready to order a monochromator. Over the next few months he expects to use the equipment and supplies budget of the DOE grant to get the supplies needed to carry out experiments at Furman. The plan is tomore » continue the summer collaboration at LANL and carry out experiments at Furman during the academic year.'« less
  • 'The author is engaged in a collaborative research effort with Los Alamos staff scientists Steven Buelow, Jeanne Robinson, and Bernie Foy all staff members in group CST-6. The work proposed by these LANL staff scientists is directed towards the destruction of complexants and oxidation of chromium and technetium by hydrothermal processing in near critical or supercritical aqueous solutions. The work addresses two areas of investigation related to ongoing efforts at LANL: (1) kinetic studies of oxidation-reduction reactions in supercritical water; (2) measurement of physical properties of ionic solutes in supercritical water. All of the work during this first year wasmore » carried out at Los Alamos National Lab. During the Summer program at LANL all equipment and supplies were provided through Dr. Buelow''s program at LANL. The author has now set up a Raman spectroscopy lab at Furman. Using departmental funds he purchased an optical bench, a laser, and a CCD detector, and a grant from the Dreyfus Foundation assisted in the purchase of a Raman spectrometer. He is now able to carry out experiments using the Raman system at Furman. The plan is to continue the Summer collaboration at LANL and carry out experiments at Furman during the academic year.'« less
  • Current efforts are focused on the oxidative dissolution of chromium compounds found in Hanford tank waste sludge. Samples of chromium oxides and hydroxides with varying degrees of hydration are being characterized using Raman, FTIR, and XPS spectroscopic techniques. Kinetics of oxidation reactions at subcritical and supercritical temperatures are being followed by Raman spectroscopy using a high temperature stainless steel cell with diamond windows. In these reactions both hydrogen peroxide and nitrate anions are used as the oxidizing species with Cr(III) compounds and organic compounds as reducing agents.
  • We are engaged in a collaborative research effort with Los Alamos staff scientists Steven Buelow and Jeanne Robinson, staff members in group CST-6. The work proposed by these LANL staff scientists is directed towards the destruction of complexants and oxidation of chromium and technetium by hydrothermal processing in near critical or supercritical aqueous solutions. Our own work has been focused on a careful kinetic study of oxidation reactions of hydrogen peroxide with chromium hydroxide. This reaction occurs readily at ambient temperatures.
  • A multi-phase ceramic waste form is being developed at the Savannah River National Laboratory (SRNL) for treatment of secondary waste streams generated by reprocessing commercial spent nuclear. The envisioned waste stream contains a mixture of transition, alkali, alkaline earth, and lanthanide metals. Ceramic waste forms are tailored (engineered) to incorporate waste components as part of their crystal structure based on knowledge from naturally found minerals containing radioactive and non-radioactive species similar to the radionuclides of concern in wastes from fuel reprocessing. The ability to tailor ceramics to mimic naturally occurring crystals substantiates the long term stability of such crystals (ceramics)more » over geologic timescales of interest for nuclear waste immobilization [1]. A durable multi-phase ceramic waste form tailored to incorporate all the waste components has the potential to broaden the available disposal options and thus minimize the storage and disposal costs associated with aqueous reprocessing. This report summarizes results from three years of work on the IAEA Coordinated Research Project on “Processing technologies for high level waste, formulation of matrices and characterization of waste forms” (T21027), and specific task “Melt Processed Crystalline Ceramic Waste Forms for Advanced Nuclear Fuel Cycles” (17208).« less