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Gibbs free energies of formation of PCDDs: Evaluation of estimation methods and application for predicting dehalogenation pathways

Journal Article · · Environmental Toxicology and Chemistry
; ;  [1];  [2]
  1. Univ. of South Alabama, Mobile, AL (United States)
  2. Research Inst. for Agrobiology and Soil Fertility, Haren (Netherlands)

Chlorinated dioxins and related compounds are discharged to the environment from incinerators, dump sites, wastewater, and as contaminants in other products. There is a great interest in developing bioremediation techniques for the transformation of these chemicals into other chemicals that are not environmentally harmful. Gibbs free energies of formation for the ideal gas, liquid phase, and species in solution were estimated for 75 polychlorinated dibenzo-p-dioxins (PCDDs) at 298.15 K and 100,000 Pa. These values were used to calculate standard redox potentials, with H{sub 2} as the electron donor. Owing to the lack of experimental thermodynamic data for the involved chemical species, the standard-state ideal gas enthalpies of formation were evaluated by several semiempirical methods including the Modified Neglect of Diatomic Differential Overlap (MNDO), Austin Model 1 (AM1), and MNDO-Parametric Method 3 (PM3). Three different implementations of Benson`s group additivity method for estimation of ideal gas enthalpies of formation were also evaluated. As a result of the evaluation, the CHETAH program based on Benson`s group additive method was chosen for ideal gas enthalpy of formation calculations. Entropies, vapor pressure, and aqueous solubility were calculated by existing methods in order to complete the thermodynamic cycle. Calculated redox potentials indicate that chlorodioxins, including 2,3,7,8-tetrachlorodioxin, can serve as electron acceptors in anaerobic environments, at least from a thermodynamic perspective.

Sponsoring Organization:
USDOE
OSTI ID:
264295
Journal Information:
Environmental Toxicology and Chemistry, Journal Name: Environmental Toxicology and Chemistry Journal Issue: 6 Vol. 15; ISSN ETOCDK; ISSN 0730-7268
Country of Publication:
United States
Language:
English

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