BASIC ENGINEERING RESEARCH FOR D&D OF R REACTOR STORAGE POND SLUDGE: ELECTROKINETICS, CARBON DIOXIDE EXTRACTION, AND SUPERCRITICAL WATER OXIDATION Page: 4 of 76
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carbon dioxide as a cosolvent. The experimental pressures were 2,000 and 4,000 psi, and the
temperatures were 40 0C and 80 0C. These experiments showed that supercritical CO2 extraction
using ethanol as a modifier is a very promising technology for extracting chlorinated aromatics
from job control waste and other DOE matrices.
The project team also constructed a continuous-flow supercritical water oxidation
(SCWO) apparatus in which to conduct hydrothermal oxidation of PCBs. Chemical analysis was
performed with a new GC/electron capture detector system. The team conducted SCWO
screening tests with methanol as a tuning compound for the continuous-flow supercritical water
oxidation reactor. Methanol was chosen not only because it is easy to work with, but also
because the supercritical water oxidation behavior of methanol is well documented in the
literature. Hydrogen peroxide was chosen as the oxidant, as it outperforms oxygen as indicated
by the literature. The reactor has obtained conversions of methanol and PCBs in excess of 99%.
This EMSP project provided support for two Masters theses and the experimental data for
two PhD dissertations (in progress).
This research is highly relevant to the needs of DOE/EM. As indicated above, within the
entire weapons complex there are approximately 19,000 m3 of PCB-contaminated low-level
mixed waste and job control waste, and more will be generated during ongoing and future D&D
operations. The only approved disposal path is incineration, and the only approved incinerator
for this type waste, at Oak Ridge, has been shut down, perhaps permanently. This process can be
a viable, safe and relatively inexpensive alternative to incineration.
This project has produced the data necessary to understand the reaction kinetics and
thermodynamics of the technologies involved. Within two more years, the project can produce
the data necessary for prototype design and a larger-scale demonstration. Further research and
development would include (1) fine tuning the CO2/ethanol extraction process to achieve higher
rates of extraction; (2) additional lab-scale tests comparing hot water and CO2 as the extraction
solvent, and extracting PCBs from additional solid matrices of interest to SRS and DOE; (3)
performing additional experiments and kinetic analysis of the SCWO process; (4) obtaining
additional phase equilibrium data for PCBs in support of extraction and oxidation modeling; and
(5) modeling and consolidating all technical data so that a prototype combined-cycle apparatus
could be built and a larger-scale demonstration could be considered for implementation by DOE.
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Matthews, Michael A.; Bruce,David; Davis,Thomas; Thies, Mark; Weidner, John & White, Ralph. BASIC ENGINEERING RESEARCH FOR D&D OF R REACTOR STORAGE POND SLUDGE: ELECTROKINETICS, CARBON DIOXIDE EXTRACTION, AND SUPERCRITICAL WATER OXIDATION, report, December 31, 2001; United States. (digital.library.unt.edu/ark:/67531/metadc781221/m1/4/: accessed December 18, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.