In water treatment, chemical oxidation and reduction processes have been used for a number of years to treat contaminated water. For organic contaminants found in water, the purpose is to convert such contaminants into harmless or nonobjectionable forms. Several technologies that have shown promise to destroy many of the emerging organic contaminants in water are the so-called advanced oxidation processes (AOPs), which produce hydroxyl radicals (HO•) at room temperature and pressure. The HO• radical is an electrophile that reacts rapidly and non-selectively with most electron-rich organic compounds. With increasing concern about emerging contaminants and their adverse human and ecological effects, it is likely that the use of AOPs will continue to increase.
Rate Constants and Toxicity Estimation for the Computer Discovery of Byproducts Fate in Advanced Oxidation Systems
Sponsored by the National Science Foundation
This goal of this project is to develop modules to predict reaction rate constants for elementary reactions that are predicted by a previously developed computer-based reaction pathway generator and to estimate toxicity of intermediate products in aqueous phase advanced oxidation processes (AOPs). Concentration profiles of organic contaminants and intermediate products will be obtained by solving ordinary differential equations. The predicted kinetic information and toxicity can be used to identify important pathways of AOPs and these can be used to guide the design of experiments that are used to examine the reaction mechanisms of important byproducts. This project will help researchers and engineers gain a quantitative insight of hydroxyl radical induced reactions, and provide important information for quantifying the efficacy of AOPs as alternative water treatment processes.
- Yao, H.; Sun, P.; Minakata, D.; Crittenden, J.C.; Huang, C-H.; "Kinetics and Modeling of Degradation of Ionophore Antibiotics by UV and UV/H2O2," Environ. Sci. Technol., 2013, (47) 4581-4589. Abstract
- Minakata, D.; Song, W.; Crittenden, J.; "Reactivity of aqueous phase hydroxyl radical with halogenated carboxylate anions: Experimental and theoretical studies," Environ. Sci. & Technol. 2011, 45, 6057-6065. Abstract
- Minakata, D.; Crittenden, J.,"Linear Free Energy Relationships between the Aqueous Phase Hydroxyl Radical (HO•) Reaction Rate Constants and the Free Energy of Activation.," Environ. Sci. & Technol. 2011, 45, 3479-3486. Abstract
- Westerhoff, Paul; Moon, Hye; Minakata, Daisuke; Crittenden, John, “Oxidation of Organics in Retentates from Reverse Osmosis Wastewater Reuse Facilities,” Water Research, 43 (16): 3992-2998 Sp. Iss. SI SEP 2009.
- Minakata, Daisuke; Li, Ke; Westerhoff, Paul; Crittenden, John, “Development of a Group Contribution Method to Predict
Phase Hydroxyl Radical (HO center dot) Reaction Rate Constants,” Environmental Science & Technology, 43 (16): 6220-6227
JUL 06 2009.
Note: Professor Hartmut Herrmann stated in his 2010 review paper that “The wide application range in combination with the user-friendliness makes it probably the best currently available estimation tool for OH radical reactions in aqueous solution." (Herrmann, et al., 2010, ChemPhysChem. 11, 3796-3822.)
- Li, K.; Crittenden, J., “Computerized Pathway Elucidation for Hydroxyl Radical-Induced Chain Reaction Mechanisms in Aqueous Phase Advanced Oxidation Processes,” Environmental Science & Technology, 43 (8): 2831-2837 APR 15 2009.
- Li, Ke; Hokanson, David R.; Crittenden, John C; Trussell, Rhodes R; Minakata, Daisuke, “Evaluating UV/H202 Processes for Methyl Tert-butyl Ether and Tertiary Butyl Alcohol Removal: Effect of Pretreatment Options and Light Sources," Water Research, 42 (20): 5045-5053 DEC 2008.
- Ke Li, David R. Hokanson, John C. Crittenden, R. Rhodes Trussell, and Daisuke Minakata, “Evaluating UV/H2O2 Processes for Methyl tert-Butyl Ether (MtBE) and 16 tertiary Butyl Alcohol (TBA) Removal from Drinking Water Source: Effect of Pretreatment Options and Light Sources," Communicated to Aqua (2007).
- Westerhoff, P.; Mezyk, S.P.; Cooper, W.J.; Minakata, D., "Electron pulse radiolysis determination of hydroxyl radical rate constants with Suwannee river fulvic acid and other dissolved organic matter isolates," Environ. Sci. & Technol. 2007, 41, 4610-4646.
- Li, K, M. I. Stefan and J. C. Crittenden, “Trichloroethene (TCE) Degradation by UV/H2O2 Advanced Oxidation Process: Product Study and Kinetic Modeling,” Environmental Science and Technology, 41:1696-1703 (2007).
- Li, K, M. I. Stefan and J. C. Crittenden, “UV Photolysis of Trichloroethylene (TCE): Product Study and Kinetic Modeling,” Environmental Science and Technology, Vol. 38, No. 24, 6685-6693(2004).
- Crittenden, John C., Shumin Hu, David W. Hand, and Sarah Green, “A Kinetic Model for H2O2/UV Process in a Completely Mixed Batch Reactor,” Water Research, 33(10), 2315-2328 (1999).
- "Mechanistic Insights in Peroxyl Radical Formation and Degradation and Associated Reaction Rate Constants Prediction in Aqueous Phase Advanced Oxidation Processes," Minakata, D.; Mezyk, S.; Jones, J. and Crittenden, J.C., ACS National Meeting in New Orleans, Louisiana, April 7, 2013. Download PDF (~3.5 MB)
- "Advanced Oxidation Processes and Biological Treatment," Crittenden, J.C.; Pavlostathis, S.; Minakata, D. Institute for Light Industry, China, December 16, 2011. Download PDF (~3.3 MB)
- "Theoretical Study in the Aqueous-Phase Subsequent Free-Radical Reactions Induced by Hydroxyl Radicals," Minakata, Crittenden, ACS National Meeting in Denver, Colorado, August 29, 2011. Download PDF (~1.2 MB)
- "Rational Design of Advanced Oxidation Processes using Computational Chemistry," Minakata, D.; Li, K.; Crittenden, J.C. GCOE Symposium, Kyoto University, Kyoto, Japan, July 21, 2011. Download PDF (~2 MB)
- "Development of Computer-based Kinetic Model for the Treatment of Emerging Contaminants in Aqueous Advanced Oxidation Processes," Minakata, D.; Crittendent, J.C.; Li, K., Georgia Tech Strategic Planning Meeting & Poster Session. Large-Scale Data and High Performance Computing. February, 2011. 1116 Klaus Advanced Computing Building, Download PDF (~.75 MB)
- "Rational Design of Advanced Oxidation Processes using Computational Chemistry," presented at AOT - 16 in San Diego, CA USA, Minakata, Li, Crittenden, and Hand, 11/15-18/2010, Download PDF (~1.47 MB)
- "Quantitative Understanding of Advanced Oxidation Processes for the Treatment of Emerging Contaminants," presented at the International Water Association World Water Congress & Exhibition in Montreal, Minakata, Crittenden, 8/24/2010, Download PDF (~0.55 MB)
- "Linear Free Energy Relationships for the Aqueous Phase Hydroxyl Radical Reaction with Ionized Species: Experimental and Theoreatical Studies," presented at the American Chemical Society Conference in Boston, MA, Minakata, Crittenden, 8/22/2010, Download PDF (~0.5 MB)
- "Overview of Advanced Oxidation Processes (AOPs) - Understanding and Improving Process Performance," presented at Potable Water Reuse Conference, Crittenden, Li, Minakata, & Westerhoff, 11/19/2008, Download PDF (~1.55 MB)
- "Development of Group Contribution Method (GCM) for Hydroxyl Radical (HO•) Reaction Rate Constants in the Aqueous Phase," presented at AOT - 14, Minakata, Li, Crittenden, & Westerhoff, 9/22/2008, Download PDF (~1 MB)
- "Understanding and Improving Process Performance of Advanced Oxidation Processes (AOPs)," presented to the Hong Kong University of Science and Technology, Crittenden, et al., 6/27/2008, Download PDF (~2.3 MB)
- "Life Cycle Assessment of Three Water Scenarios: Importation, Reclamation, and Desalination," presented at the EPRI Workshop to assess research opportunities for water use efficiency technologies, Crittenden, et al., 11/15/2007 Download PDF (~1.1 MB)
- "Evaluation and Design Advanced Oxidation Processes (AOPs)," presented at the Water Quality Technology Conference Workshops at the Sun 5 Advanced Oxidation Technologies in Water, Minakata, Crittenden, Li, Hokanson, & Trussell, 11/4/2007 Download PDF (~1.8 MB)
- "Mitigation of Bromateduring Ozonation," presented in Mexico City, Crittenden, Minakata, & Chowdhury, 9/27/2007 Download PDF (~1.5 MB)
- "UV/H2O2 Process Modeling for Design and Mechanistic Studies," presented at Developments in Drinking Water Treatment Modeling, Crittenden, Li, & Hand, 6/22/2006 Download PDF (~1.5 MB)
- "AdOx™ - a Kinetic Model for the Hydrogen Peroxide / UV Process," presented at the Sixth Annual Conference on Advanced Oxidation Technologies for Water and Air Remediation, Li, Hu, Crittenden, Hand, & Hokanson, 6/30/2000 Download PDF (~0.3 MB)
Research Engineer, BBISS
Asst. Professor, UGA
Graduate Student Asst.