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http://dx.doi.org/10.15681/KSWE.2015.31.5.468

A Study on the Degradation Properties of Aqueous Trinitrotoluene by Palladium Catalyst and Formic Acid  

Jeong, Sangjo (Department of Civil Engineering and Environmental Sciences, Korea Military Academy)
Choi, Hyungjin (Department of Civil Engineering and Environmental Sciences, Korea Military Academy)
Park, Sangjin (Department of Civil Engineering and Environmental Sciences, Korea Military Academy)
Lee, Juneil (Department of Civil Engineering and Environmental Sciences, Korea Military Academy)
Publication Information
Journal of Korean Society on Water Environment / v.31, no.5, 2015 , pp. 468-475 More about this Journal
Abstract
Various methods to degrade explosives efficiently in natural soil and water that include trinitrotoluene (TNT) have been studied. In this study, TNT in water was degraded by reduction with palladium (Pd) catalyst impregnated onto alumina (henceforth Pd-Al catalyst) and formic acid. The degradation of TNT was faster when the temperature of water was high, and the initial TNT concentration, pH, and ion concentration in water were low. The amounts of Pd-Al catalyst and formic acid were also important for TNT degradation in water. According to the experimental results, the degradation constant of TNT with unit mass of Pd-Al catalyst was $8.37min^{-1}g^{-1}$. The degradation constant of TNT was higher than the results of previous studies which used zero valent iron. 2,6-diamino-4-nitrotoluene and 2-amino-4,6-dinitrotoluene were detected as by-products of TNT degradation showing that TNT was reduced. The by-products of TNT were also completely degraded after reaction when both Pd-Al catalyst and formic acid existed. Even though there are several challenges of Pd-Al catalyst (e.g., deactivation, poisoning, leaching, etc.), the results of this study show that TNT degradation by Pd-Al catalyst and formic acid is a promising technique to remediate explosive contaminated water and soil.
Keywords
Catalyst; Degradation; Formic acid; Palladium; Trinitrotoluene;
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Times Cited By KSCI : 2  (Citation Analysis)
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1 Ayoub, K., Nelieu, S., van Hullebusch, E. D., Maia-Grondard, A., Cassir, M., and Bermond, A. (2011). TNT Oxidation by Fenton Reaction: Reagent Ratio Effect on Kinetics and Early Stage Degradation Pathways, Chemical Engineering Journal, 173, pp. 309-317.   DOI
2 Ayoub, K., van Hullebusch, E., Cassir, M., and Bermond, A. (2010). Application of Advanced Oxidation Processes for TNT Removal: A Review, Journal of Hazardous Materials, 178, pp. 10-28.   DOI   ScienceOn
3 Bae, B. (2006). Reduction of High Explosives (HMX, RDX, and TNT) Using Micro- and Nano- Size Zero Valent Iron: Comparison of Kinetic Constants and Intermediates Behavior, Journal of Soil and Groundwater Environment, 11, pp. 83-91.
4 Bae, B., and Park, J. (2014). Distribution and Migration Characteristics of Explosive Compounds in Soil at Military Shooting Ranges in Gyeonggi Province, Journal of the Korean Geo-Environmental Society, 15, pp. 17-29.
5 Banas, A., Banas, K., Bahou, M., Moser, H., Wen, L., Yang, P., Li, Z., Cholewa, M., Lim, S., and Lim, C. (2009). Post-blast Detection of Traces of Explosives by Means of Fourier Transform Infrared Spectroscopy, Vibrational Spectroscopy, 51, pp. 168-176.   DOI
6 Brannon, J., Jenkins, T., Parker, L., Deliman, P., Gerald, J., Ruiz, C., Porter, B., and Davis, W. (2000). Procedures for Determining Integrity of UXO and Explosives Soil Contamination at Firing Ranges (No. ERDC-TR-00-4), U.S. Army Enigieer Research and Development Center.
7 Chen, W., Juan, C., and Wei, K. (2005). Mineralization of Dinitrotoluenes and Trinitrotoluene of Spent Acid in Toluene Nitration Process by Fenton Oxidation, Chemosphere, 60, pp. 1072-1079.   DOI
8 Chen, W., Juan, C., and Wei, K. (2007). Decomposition of Dinitrotoluene Isomers and 2,4,6-trinitrotoluene in Spent Acid from Toluene Nitration Process by Ozonation and Photoozonation, Journal of Hazardous Materials, 147, pp. 97-104.   DOI
9 Cho, C., Bae, S., and Lee, W. (2012). Enhanced Degradation of TNT and RDX by Bio-reduced Iron Bearing Soil Minerals, Advances in Environmental Research, 1, pp. 1-14.   DOI   ScienceOn
10 Dillert, R., Fornefett, I., Siebers, U., and Bahnemann, D. (1996). Photocatalytic Degradation of Trinitrotoluene and Trinitrobenzene: Influence of Hydrogen Peroxide, Journal of Photochemistry and Photobiology A: Chemistry, 94, pp. 231-236.   DOI
11 Elovitz, M. and Weber, E. (1999). Sediment-Mediated Reduction of 2,4,6-trinitrotoluene and Fate of the Resulting Aromatic (Poly)amines, Environmental Science & Technology, 33, pp. 2617-2625.   DOI
12 Hess, T., Lewis, T., Crawford, R., Katamneni, S., Wells, J., and Watts, R. (1998). Combined Photocatalytic and Fungal Treatment for the Destruction of 2,4,6-trinitrotoluene (TNT), Water Research, 32, pp. 1481-1491.   DOI
13 Kalderis, D., Juhasz, A., Boopathy, R., and Comfort, S. (2011). Soils Contaminated with Explosives: Environmental Fate and Evaluation of State-of-the-art Remediation Processes, Pure and Applied Chemistry, 83, pp. 1407-1484.
14 Hoffmann, M., Hua, I., and Hochemer, R. (1996). Application of Ultrasonic Irradiation for the Degradation of Chemical Contaminants in Water, Ultrasonics Sonochemistry, 3, pp. S163-S172.   DOI   ScienceOn
15 Hundal, L., Singh, J., Bier, E., Shea, P., Comfort, S., and Powers, W. (1997). Removal of TNT and RDX from Water and Soil Using Iron Metal, Environmental Pollution, 97, pp. 55-64.   DOI
16 Jung, H. (2004). Removal of 2,4,6-trinitrotoluene by Oxidant Reductant Treatment Process, Master's Thesis, Kyungpook National University.
17 Kim, S., Back, K., Lee, I., Bae, B., and Chang, Y. (2002). A Column Study on Phytoremediation of 2,4,6-trinitrotoluene (TNT) Contaminated Soil, Journal of Korean Society of Environmental Engineers, 24, pp. 2039-2046.
18 Kwon, B., Choi, W., and Yoon, J. (2010). Photo Decomposition Characteristics of 2,4,6-trinitrotoluene in a UV/$H_2O_2$ Process, Journal of Korean Society of Water and Wastewater, 24, pp. 775-788.
19 Kwon, Y., Kim, D., Jeong, Y., Bae, B., Lee, I., and Jang, Y. (2004). Romoval of 2,4,6-trinitrotoluene(TNT) by Indigenous Grasses, Abutilon Avicennae and Aeschynomene Indica, in Hydroponic Culture, Journal of Korean Society on Water Quality, 20, pp. 32-36.
20 Lee, B., and Jeong, S. (2009). Effects of Additives on 2,4,6-trinitrotoluene (TNT) Removal and Its Mineralization in Aqueous Solution by Gamma Irradiation, Journal of Hazardous Materials, 165, pp. 435-440.   DOI
21 Lowry, G. and Reinhard, M. (1999). Hydrodehalogenation of 1-to 3-carbon Halogenated Organic Compounds in Water Using a Palladium Catalyst and Hydrogen Gas, Environmental Science & Technology, 33, pp. 1905-1910.   DOI
22 Lee, B. and Lee, M. (2005). Decomposition of 2,4,6-trinitrotoluene (TNT) by Gamma Ray Irradiation, Journal of Korean Society of Environmental Engineers, 27, pp. 1-10.
23 Li, Z., Shea, P., and Comfort, S. (1998). Nitrotoluene Destruction by UV-catalyzed Fenton Oxidation, Chemosphere, 36, pp. 1849-1865.   DOI
24 Liou, M., Lu, M., and Chen, J. (2004). Oxidation of TNT by Photo-Fenton Process, Chemosphere, 57, pp. 1107-1114.   DOI
25 Matta, R., Hanna, K., and Chiron, S. (2007). Fenton-like Oxidation of 2,4,6-trinitrotoluene Using Different Iron Minerals, Science of The Total Environment, 385, pp. 242-251.   DOI
26 Mese, S. and Lehmpuhl, D. (2008). Hydrogen Donors for Reduction of RDX, 2, 4-DNT, and Nitrate in Groundwater, Soil & Sediment Contamination, 17, pp. 505-515.   DOI
27 Nasri, N., Tatt, E., Hamza, U., Mohammed, J., and Zain, H. (2015). Kinetic Rate Comparison of Methane Catalytic Combustion of Palladium Catalysts Impregnated onto r-Alumina and Bio-char, International Scholarly and Scientific Research & Innovation, 9, pp. 531-537.
28 Ro, K., Venugopal, A., Adrian, D., Constant, D., Qaisi, K., Valsaraj, K., Thibodeaux, L., and Roy, D. (1996). Solubility of 2,4,6-trinitrotoluene (TNT) in Water, Journal of Chemical & Engineering Data, 41, pp. 758-761.   DOI
29 Shin, G. and Kim, Y. (2002). Photocatalytic Degradation of 2,4,6-trinitrotoluene (TNT) in a $TiO_2$ Thin Film Reactor, Journal of the Korean Society of Water and Wastewater, 16, pp. 145-152.
30 Smith, R., Miller, D., Brooks, M., Widdowson, M., and Killingstad, M. (2001). In Situ Stimulation of Groundwater Denitrification with Formate to Remediate Nitrate Contamination, Environmental Science & Technology, 35, pp. 196-203.   DOI
31 Son, H., Lee, S., Cho, I., and Zoh, K. (2004). Kinetics and Mechanism of TNT Degradation in $TiO_2$ Photocatalysis, Chemosphere, 57, pp. 309-317.   DOI
32 Sriwatanapongse, W. (2005). Reductive Dechlorination of Trichloroethylene by Palladium on Alumina Catalyst: a Solid-State NMR Study of Surface Reaction Mechanism, Ph.D. Dissertation, Stanford University.
33 U.S. EPA. (2012). 2012 Edition of the Drinking Water Standards and Health Advisories.
34 Wei, F., Zhang, Y., Lv, F., Chu, P., and Ye, Z. (2011). Extraction of Organic Materials from Red Water by Metal-impregnated Lignite Activated Carbon, Journal of Hazardous Materials, 197, pp. 352-360.   DOI
35 Zhang, M., Zhao, Q., and Ye, Z. (2011). Organic Pollutants Removal from 2,4,6-trinitrotoluene (TNT) Red Water Using Low Cost Activated Coke, Journal of Environmental Sciences, 23, pp. 1962-1969.   DOI
36 Zhang, X., Lin, Y., Shan, X., and Chen, Z. (2010). Degradation of 2,4,6-trinitrotoluene (TNT) from Explosive Wastewater Using Nanoscale Zero-valent Iron, Chemical Engineering Journal, 158, pp. 566-570.   DOI