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Title: High energy decomposition of halogenated hydrocarbons. FY 1992 final report

Abstract

This program is the INEL component of a joint collaborative effort with Lawrence Livermore National Laboratory (LLNL). Purpose is to demonstrate a viable process for breaking down hazardous halogenated organic wastes to simpler, nonhazardous wastes using high energy ionizing radiation. The INEL effort focuses on the use of spent reactor fuel gamma radiation sources to decompose complex wastes such as PCBS. Work in FY92 expanded upon that reported for FY91. During FY91 it was reported that PCBs were susceptible to radiolytic decomposition in alcoholic solution, but that only a small percentage of decomposition products could be accounted for. It was shown that decomposition was more efficient in methanol than in isopropanol and that the presence of a copper-zinc couple catalyst did not affect the reaction rate. Major goals of FY92 work were to determine the reaction mechanism, to identify further reaction products, and to select a more appropriate catalyst. Described in this report are results of mechanism specific experiments, mass balance studies, transformer oil irradiations, the use of hydrogen peroxide as a potential catalyst, and the irradiation of pure PCB crystals in the absence of diluent.

Authors:
; ;
Publication Date:
Research Org.:
EG and G Idaho, Inc., Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10116942
Report Number(s):
EGG-PHY-10446
ON: DE93005268
DOE Contract Number:
AC07-76ID01570
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: Sep 1992
Country of Publication:
United States
Language:
English
Subject:
07 ISOTOPES AND RADIATION SOURCES; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; CHLORINATED AROMATIC HYDROCARBONS; RADIOLYSIS; PROGRESS REPORT; GAMMA RADIATION; SPENT FUELS; METHANOL; PROPANOLS; CARBON TETRACHLORIDE; WASTE PROCESSING; CHEMICAL REACTION KINETICS; TRANSFORMERS; INSULATING OILS; 070205; 400600; 320305; INDUSTRIAL APPLICATIONS, RADIATION PROCESSING; RADIATION CHEMISTRY; INDUSTRIAL WASTE MANAGEMENT

Citation Formats

Mincher, B.J., Arbon, R.E., and Meikrantz, D.H. High energy decomposition of halogenated hydrocarbons. FY 1992 final report. United States: N. p., 1992. Web. doi:10.2172/10116942.
Mincher, B.J., Arbon, R.E., & Meikrantz, D.H. High energy decomposition of halogenated hydrocarbons. FY 1992 final report. United States. doi:10.2172/10116942.
Mincher, B.J., Arbon, R.E., and Meikrantz, D.H. 1992. "High energy decomposition of halogenated hydrocarbons. FY 1992 final report". United States. doi:10.2172/10116942. https://www.osti.gov/servlets/purl/10116942.
@article{osti_10116942,
title = {High energy decomposition of halogenated hydrocarbons. FY 1992 final report},
author = {Mincher, B.J. and Arbon, R.E. and Meikrantz, D.H.},
abstractNote = {This program is the INEL component of a joint collaborative effort with Lawrence Livermore National Laboratory (LLNL). Purpose is to demonstrate a viable process for breaking down hazardous halogenated organic wastes to simpler, nonhazardous wastes using high energy ionizing radiation. The INEL effort focuses on the use of spent reactor fuel gamma radiation sources to decompose complex wastes such as PCBS. Work in FY92 expanded upon that reported for FY91. During FY91 it was reported that PCBs were susceptible to radiolytic decomposition in alcoholic solution, but that only a small percentage of decomposition products could be accounted for. It was shown that decomposition was more efficient in methanol than in isopropanol and that the presence of a copper-zinc couple catalyst did not affect the reaction rate. Major goals of FY92 work were to determine the reaction mechanism, to identify further reaction products, and to select a more appropriate catalyst. Described in this report are results of mechanism specific experiments, mass balance studies, transformer oil irradiations, the use of hydrogen peroxide as a potential catalyst, and the irradiation of pure PCB crystals in the absence of diluent.},
doi = {10.2172/10116942},
journal = {},
number = ,
volume = ,
place = {United States},
year = 1992,
month = 9
}

Technical Report:

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  • The purpose of this program is to demonstrate a viable process for the decomposition of hazardous organochlorine compounds to nonhazardous products. This process has applicability to the treatment of mixed wastes containing both chlorinated hydrocarbons and radioactive constituents. The organics may be decomposed leaving only the radioactive constituents in the waste. Further, the use of spent nuclear fuel as a gamma-ray source presents a potentially cost effective energy source and elegantly allows the fuel to be considered a resource rather than a liability. During FY93 more than 400 samples were irradiated with fission product gamma-rays. Many of these samples weremore » individual PCB congeners dissolved in isopropanol. These samples were studied to gain an understanding of the mechanism and kinetics of, and to provide a mass balance for, the PCB radiolysis reaction. In addition to research findings this report also contains a summary of efforts expended on technology transfer, professional publications and conference presentations.« less
  • This program is the INEL component of a joint collaborative effort with Lawrence Livermore National Laboratory (LLNL). Purpose is to demonstrate a viable process for breaking down hazardous halogenated organic wastes to simpler, nonhazardous wastes using high energy ionizing radiation. The INEL effort focuses on the use of spent reactor fuel gamma radiation sources to decompose complex wastes such as PCBS. Work in FY92 expanded upon that reported for FY91. During FY91 it was reported that PCBs were susceptible to radiolytic decomposition in alcoholic solution, but that only a small percentage of decomposition products could be accounted for. It wasmore » shown that decomposition was more efficient in methanol than in isopropanol and that the presence of a copper-zinc couple catalyst did not affect the reaction rate. Major goals of FY92 work were to determine the reaction mechanism, to identify further reaction products, and to select a more appropriate catalyst. Described in this report are results of mechanism specific experiments, mass balance studies, transformer oil irradiations, the use of hydrogen peroxide as a potential catalyst, and the irradiation of pure PCB crystals in the absence of diluent.« less
  • The purpose of this effort is to demonstrate a viable process for breaking down hazardous halogenated organic wastes to simpler, non-hazardous wastes using high energy ionizing radiation. The INEL effort focuses on the use of spent reactor fuel gamma radiation sources to decompose complex wastes such as PCBs. The INEL irradiation experiments concentrated on a single PCB congener so that a limited set of decomposition reactions could be studied. The congener 1, 2{prime}, 3, 3{prime}, 4, 5{prime}, 6, 6{prime} - octachlorobiphenyl was examined followed exposure to various gamma doses at the ATR spent fuel pool. The decomposition rates and productsmore » in several solvents are discussed. 7 refs., 5 figs., 3 tabs.« less
  • Anaerobic microbial transformation of monoaromatic hydrocarbons (NM), chlorinated benzenes (CB), and mixtures of MAH and CB, as well as MAH and chlorinated aliphatic solvents (tetrachloroethylene -- PCE, and carbon tetrachloride -CT) was studied in laboratory microcosms derived from hydrocarbon-contaminated groundwater aquifers. Some MAH , such as toluene and o-xylene, were completely degraded to CO 2 and CH by mixed methanogenic cultures from a creosote-contaminated aquifer. This degradation was inhibited by the addition of accessory electron acceptors (oxygen, nitrate, sulfate), indicating acclimation of the microbial community to methanogenic conditions. The addition of preferred substrates, such as acetate, propionate, methanol, fatty acids,more » glucose, casamino acids, pepton, yeast extract, or acetone also inhibited MAH degradation, indicating that the presence of natural organic substrates may preclude anaerobic biodegradation of in situ. Cyclohexane, CT, and high concentrations of toluene and o-xylene had a toxic effect. Under sulfate-reducing conditions, several MAH -- toluene, all three xylene isomers, and benzene were mineralized to CO by microorganisms from a petroleum-contaminated, sulfidogenic aquifer. Whereas 2 toluene and xylenes were sequentially degraded in a mixture, benzene was degraded only if alone, or slowly transformed in a mixture with toluene. This explains previously reported recalcitrance of benzene under anaerobic conditions. The addition of preferred substrates (lactate, glucose, or yeast extract) to the cultures temporarily inhibited the degradation of MAH. Methanogenic microcosms from the creosote-contaminated aquifer reductively dechlorinated hexa-, penta-, tetra-, tri-, and di-chlorobenzene.« less
  • The Clean Air Act Amendments of 1990, Title III, present a need for stationary source sampling and analytical methods for the list of 189 compounds. EPA has used Volatile Organic Sampling Train (VOST) and Semivolatile Organic Sampling Train (SemiVOST) sampling and analytical methods for the type of sampling of organic compounds in the past, but these methodologies have been completely validated for only a few of the organic compounds. In the study, the applicability of VOST and SemiVOST techniques to Clean Air Act halogenated compounds has been evaluated under laboratory conditions. The methods were evaluated first to determine whether themore » compounds could be analyzed successfully. The report presents the results of the laboratory experiments.« less