Evaluation of Nanoscale Zero-valent Iron for Reductive Degradation of Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX): Batch and Column Scale Studies

doi:10.7857/JSGE.2015.20.6.117

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2015 Vol.20, Issue 6 Preview Page Next Page

Evaluation of Nanoscale Zero-valent Iron for Reductive Degradation of Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX): Batch and Column Scale Studies Hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX)의 환원적 분해를 위한나노영가철의 성능평가: 회분식 및 칼럼 실험: 이충섭;오다솜;조성희;이진욱;장윤석;
Lee, Chung-Seop;Oh, Da-Som;Cho, Sung-Heui;Lee, Jin-Wook;Chang, Yoon-Seok;

30 November 2015. pp. 117 ~ 126

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Abstract

Reductive degradation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) by nanoscale zero-valent iron (nZVI) was investigated to evaluate the feasibility of using it for in-situ groundwater remediation. Batch experiments were conducted to quantify the kinetics and efficiency of RDX removal by nZVI, and to determine the effects of pH, dissolved oxygen (DO), and ionic strength on this process. Experimental results showed that the reduction of RDX by nZVI followed pseudo-first order kinetics with the observed rate constant (k_obs) in the range of 0.0056-0.0192 min⁻¹. Column tests were conducted to quantify the removal of RDX by nZVI under real groundwater conditions and evaluate the potential efficacy of nZVI for this purpose in real conditions. In column experiment, RDX removal capacity of nZVI was determined to be 82,500 mg/kg nZVI. pH, oxidation-reduction potential (ORP), and DO concentration varied significantly during the column experiments; the occurrence of these changes suggests that monitoring these quantities may be useful in evaluation of the reactivity of nZVI, because the most critical mechanisms for RDX removal are based on the chemical reduction reactions. These results revealed that nZVI can significantly degrade RDX and that use of nZVI could be an effective method for in-situ remediation of RDX-contaminated groundwater.

Keywords

Nanoscale Zero-Valent Iron;RDX;Column;Groundwater;Reduction;

References

Agrawal, A. and Tratnyek, P.G., 1996, Reduction of nitro aromatic compounds by zero-valent iron metal, Environ. Sci. Technol., 30(1), 153-160.10.1021/es950211h
Brannon, J.M., Price, C.B., Yost, S.L., Hayes, C., and Porter, B., 2005, Comparison of environmental fate and transport process descriptors of explosives in saline and freshwater systems, Mar. Pollut. Bull., 50(3), 247-251.10.1016/j.marpolbul.2004.10.008
Cho, C.-H., Bae, S.-J., and Lee, W.-J., 2012, Enhanced Degradation of TNT and RDX by Bio-reduced Iron Bearing Soil Minerals, Adv. Environ. Res., 1(1), 1-1410.12989/aer.2012.1.1.001
Cook, S.M., 2009, Assessing the Use and Application of Zero-Valent Iron Nanoparticle Technology for Remediation at Contaminated Sites, US Environmental Protection Agency.
Davis, J.L., Wani, A.H., O’Neal, B.R., and Hansen, L.D, 2004, RDX biodegradation column study: comparison of electron donors for biologically induced reductive transformation in groundwater, J. Hazard. Mater., 112(1-2), 45-54.10.1016/j.jhazmat.2004.03.020
Dombek, T., Dolan, E., Schultz, J., and Klarup, D., 2001, Rapid reductive dechlorination of atrazine by zero-valent iron under acidic conditions, Environ. Pollut., 111(1), 21-27.10.1016/S0269-7491(00)00033-6
Eisentraeger, A., Reifferscheid, G., Dardenne, F., Blust, R., and Schofer, A, 2007, Hazard characterization and identification of a former ammunition site using microarrays, bioassays, and chemical analysis, Environ. Toxicol. Chem., 26(4), 634-646.10.1897/06-285R.1
Gavaskar, A., Tatar, L., and Condit W., 2005, Cost and Performance Report Nanoscale Zero-Valent Iron Technologies for Source Remediation, Cost and Performance Report: Naval Facilities Engineering Service Center: Port Hueneme, CA, 2005.
Gong, J., Lee, C.-S., Chang, Y.-Y., and Chang, Y.-S., 2015, Novel self-assembled bimetallic structure of Bi/Fe⁰ : the oxidative and reductive degradation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX), J. Hazard. Mater., 286, 107-117.10.1016/j.jhazmat.2014.10.063
Hawari, J., Halasz, A., Groom, C., Deschamps, S., Paquet, L., Beaulieu, C., and Corriveau, A, 2002, Photodegradation of RDX in aqueous solution: A mechanistic probe for biodegradation with Rhodococcus sp., Environ. Sci. Technol., 36(23), 5117-5123.10.1021/es0207753
Kaplan, D.L., 1992, Biological degradation of explosives and chemical agents, Curr. Opin. Biotech., 3(3), 253-260.10.1016/0958-1669(92)90100-W
Kim, E.-J., Murugesan, K., Kim, J.-H., Tratnyek, P.G., and Chang, Y.-S., 2013, Remediation of Trichloroethylene by FeS-Coated Iron Nanoparticles in Simulated and Real Groundwater: Effects of Water Chemistry, Ind. Eng. Chem. Res., 52(27), 9343-9350.10.1021/ie400165a
Koutsospyros, A., Pavlov, J., Fawcett, J., Strickland, D., Smolinski, B., and Braida, W., 2012, Degradation of high energetic and insensitive munitions compounds by Fe/Cu bimetal reduction, J. Hazard. Mater., 219-220, 75-81.10.1016/j.jhazmat.2012.03.048
Liu, Y. and Lowry, G.V., 2006, Effect of particle age (Fe⁰ content) and solution pH on NZVI reactivity: H₂ evolution and TCE dechlorination, Environ. Sci. Technol., 40(19), 6085-6090.10.1021/es060685o
Lv, X., Hu, Y., Tang, J., Sheng, T., Jiang, G., and Xu, X., 2013, Effects of co-existing ions and natural organic matter on removal of chromium (VI) from aqueous solution by nanoscale zero valent iron (nZVI)-Fe₃O₄ nanocomposites, Chem. Eng. J., 218, 55-64.10.1016/j.cej.2012.12.026
Naja, G., Halasz, A., Thiboutot, S., Ampleman, G., and Hawari, J., 2008, Degradation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) using zerovalent iron nanoparticles, Environ. Sci. Technol., 42(12), 4364-4370.10.1021/es7028153
Oh, S.-Y., Cha, D.-K., Kim, B.-J., and Chiu, P.C., 2005, Reductive transformation of hexahydro-1,3,5-trinitro-1,3,5-triazine, octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine, and methylenedinitramine with elemental iron, Environ. Toxicol. Chem., 24(11), 2812-2819.10.1897/04-662R.1
Oh, S.-Y., Chiu, P.C., Kim, B.-J., and Cha, D.-K., 2003, Enhancing Fenton oxidation of TNT and RDX through pretreatment with zero-valent iron, Water Res., 37(17), 4275-4283.10.1016/S0043-1354(03)00343-9
Robidoux, P.Y., Svendsen, C., Caumartin, J., Hawari, J., Ampleman, G., Thiboutot, S., Weeks, J.M., and Sunahara, G.I., 2000, Chronic toxicity of energetic compounds in soil determined using the earthworm (Eisenia andrei) reproduction test, Environ. Toxicol. Chem., 19(7), 1764-1773.10.1002/etc.5620190709
Rosenblatt, D.H., Burrows, E.P., Mitchell, W.R., and Parmer, D.L., 1991, Organic Explosives and Related Compounds, The Handbook of Environmental Chemistry, Volume 3, Part G, Hutzinger, O. (Ed.), Springer-Verlag, Berlin.
Saleh, N., Kim, H.J., Phenrat, T., Matyjaszewski, K., Tilton, R.D., and Lowry, G.V., 2008, Ionic strength and composition affect the mobility of surface-modified Fe⁰ nanoparticles in water-saturated sand columns, Environ. Sci. Technol., 42(9), 3349-3355.10.1021/es071936b
Sun, Y.-P., Li, X.-Q., Zhang, W.-X., and Wang, H.P., 2007, A method for the preparation of stable dispersion of zero-valent iron nanoparticles, Colloid Surf. A-Physicochem. Eng. Asp., 308(1-3), 60-66.10.1016/j.colsurfa.2007.05.029
U.S. Army, 1983, Environmental fate studies on certain munitions wastewater constituents: Phase IV-Lagoon model studies.
USEPA, 2012, Drinking Water Standards and Health Advisories.
Wanaratna, P., Christodoulatos, C., and Sidhoum, M., 2006, Kinetics of RDX degradation by zero-valent iron (ZVI), J. Hazard. Mater., 136(1), 68-74.10.1016/j.jhazmat.2005.11.015
Wei, Y.-T., Wu, S.-C., Chou, C.-M., Che, C.-H., Tsai, S.-M., and Lien, H.-L., 2010, Influence of nanoscale zero-valent iron on geochemical properties of groundwater and vinyl chloride degradation: A field case study, Water Res., 44(1), 131-140.10.1016/j.watres.2009.09.012
Yu, R.-F., Chi, F.-H., Cheng, W.-P., and Chang, J.-C., 2014, Application of pH, ORP, and DO monitoring to evaluate chromium(VI) removal from wastewater by the nanoscale zero-valent iron (nZVI) process, Chem. Eng. J., 255, 568-576.10.1016/j.cej.2014.06.002
Zhang, W.-X. and Elliott, D.W., 2006, Applications of iron nanoparticles for groundwater remediation, Remediati. J., 16(2), 7-21.10.1002/rem.20078

Information

Publisher :The Korean Society of Soil and Groundwater Environment
Publisher(Ko) :한국지하수토양환경학회
Journal Title :Journal of Soil and Groundwater Environment
Journal Title(Ko) :지하수토양환경
Volume : 20
No :6
Pages :117 ~ 126
DOI :https://doi.org/10.7857/JSGE.2015.20.6.117

[1] Agrawal, A. and Tratnyek, P.G., 1996, Reduction of nitro aromatic compounds by zero-valent iron metal, Environ. Sci. Technol., 30(1), 153-160.10.1021/es950211h

[2] Brannon, J.M., Price, C.B., Yost, S.L., Hayes, C., and Porter, B., 2005, Comparison of environmental fate and transport process descriptors of explosives in saline and freshwater systems, Mar. Pollut. Bull., 50(3), 247-251.10.1016/j.marpolbul.2004.10.008

[3] Cho, C.-H., Bae, S.-J., and Lee, W.-J., 2012, Enhanced Degradation of TNT and RDX by Bio-reduced Iron Bearing Soil Minerals, Adv. Environ. Res., 1(1), 1-1410.12989/aer.2012.1.1.001

[4] Cook, S.M., 2009, Assessing the Use and Application of Zero-Valent Iron Nanoparticle Technology for Remediation at Contaminated Sites, US Environmental Protection Agency.

[5] Davis, J.L., Wani, A.H., O’Neal, B.R., and Hansen, L.D, 2004, RDX biodegradation column study: comparison of electron donors for biologically induced reductive transformation in groundwater, J. Hazard. Mater., 112(1-2), 45-54.10.1016/j.jhazmat.2004.03.020

[6] Dombek, T., Dolan, E., Schultz, J., and Klarup, D., 2001, Rapid reductive dechlorination of atrazine by zero-valent iron under acidic conditions, Environ. Pollut., 111(1), 21-27.10.1016/S0269-7491(00)00033-6

[7] Eisentraeger, A., Reifferscheid, G., Dardenne, F., Blust, R., and Schofer, A, 2007, Hazard characterization and identification of a former ammunition site using microarrays, bioassays, and chemical analysis, Environ. Toxicol. Chem., 26(4), 634-646.10.1897/06-285R.1

[8] Gavaskar, A., Tatar, L., and Condit W., 2005, Cost and Performance Report Nanoscale Zero-Valent Iron Technologies for Source Remediation, Cost and Performance Report: Naval Facilities Engineering Service Center: Port Hueneme, CA, 2005.

[9] Gong, J., Lee, C.-S., Chang, Y.-Y., and Chang, Y.-S., 2015, Novel self-assembled bimetallic structure of Bi/Fe⁰ : the oxidative and reductive degradation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX), J. Hazard. Mater., 286, 107-117.10.1016/j.jhazmat.2014.10.063

[10] Hawari, J., Halasz, A., Groom, C., Deschamps, S., Paquet, L., Beaulieu, C., and Corriveau, A, 2002, Photodegradation of RDX in aqueous solution: A mechanistic probe for biodegradation with Rhodococcus sp., Environ. Sci. Technol., 36(23), 5117-5123.10.1021/es0207753

[11] Kaplan, D.L., 1992, Biological degradation of explosives and chemical agents, Curr. Opin. Biotech., 3(3), 253-260.10.1016/0958-1669(92)90100-W

[12] Kim, E.-J., Murugesan, K., Kim, J.-H., Tratnyek, P.G., and Chang, Y.-S., 2013, Remediation of Trichloroethylene by FeS-Coated Iron Nanoparticles in Simulated and Real Groundwater: Effects of Water Chemistry, Ind. Eng. Chem. Res., 52(27), 9343-9350.10.1021/ie400165a

[13] Koutsospyros, A., Pavlov, J., Fawcett, J., Strickland, D., Smolinski, B., and Braida, W., 2012, Degradation of high energetic and insensitive munitions compounds by Fe/Cu bimetal reduction, J. Hazard. Mater., 219-220, 75-81.10.1016/j.jhazmat.2012.03.048

[14] Liu, Y. and Lowry, G.V., 2006, Effect of particle age (Fe⁰ content) and solution pH on NZVI reactivity: H₂ evolution and TCE dechlorination, Environ. Sci. Technol., 40(19), 6085-6090.10.1021/es060685o

[15] Lv, X., Hu, Y., Tang, J., Sheng, T., Jiang, G., and Xu, X., 2013, Effects of co-existing ions and natural organic matter on removal of chromium (VI) from aqueous solution by nanoscale zero valent iron (nZVI)-Fe₃O₄ nanocomposites, Chem. Eng. J., 218, 55-64.10.1016/j.cej.2012.12.026

[16] Naja, G., Halasz, A., Thiboutot, S., Ampleman, G., and Hawari, J., 2008, Degradation of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) using zerovalent iron nanoparticles, Environ. Sci. Technol., 42(12), 4364-4370.10.1021/es7028153

[17] Oh, S.-Y., Cha, D.-K., Kim, B.-J., and Chiu, P.C., 2005, Reductive transformation of hexahydro-1,3,5-trinitro-1,3,5-triazine, octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine, and methylenedinitramine with elemental iron, Environ. Toxicol. Chem., 24(11), 2812-2819.10.1897/04-662R.1

[18] Oh, S.-Y., Chiu, P.C., Kim, B.-J., and Cha, D.-K., 2003, Enhancing Fenton oxidation of TNT and RDX through pretreatment with zero-valent iron, Water Res., 37(17), 4275-4283.10.1016/S0043-1354(03)00343-9

[19] Robidoux, P.Y., Svendsen, C., Caumartin, J., Hawari, J., Ampleman, G., Thiboutot, S., Weeks, J.M., and Sunahara, G.I., 2000, Chronic toxicity of energetic compounds in soil determined using the earthworm (Eisenia andrei) reproduction test, Environ. Toxicol. Chem., 19(7), 1764-1773.10.1002/etc.5620190709

[20] Rosenblatt, D.H., Burrows, E.P., Mitchell, W.R., and Parmer, D.L., 1991, Organic Explosives and Related Compounds, The Handbook of Environmental Chemistry, Volume 3, Part G, Hutzinger, O. (Ed.), Springer-Verlag, Berlin.

[21] Saleh, N., Kim, H.J., Phenrat, T., Matyjaszewski, K., Tilton, R.D., and Lowry, G.V., 2008, Ionic strength and composition affect the mobility of surface-modified Fe⁰ nanoparticles in water-saturated sand columns, Environ. Sci. Technol., 42(9), 3349-3355.10.1021/es071936b

[22] Sun, Y.-P., Li, X.-Q., Zhang, W.-X., and Wang, H.P., 2007, A method for the preparation of stable dispersion of zero-valent iron nanoparticles, Colloid Surf. A-Physicochem. Eng. Asp., 308(1-3), 60-66.10.1016/j.colsurfa.2007.05.029

[23] U.S. Army, 1983, Environmental fate studies on certain munitions wastewater constituents: Phase IV-Lagoon model studies.

[24] USEPA, 2012, Drinking Water Standards and Health Advisories.

[25] Wanaratna, P., Christodoulatos, C., and Sidhoum, M., 2006, Kinetics of RDX degradation by zero-valent iron (ZVI), J. Hazard. Mater., 136(1), 68-74.10.1016/j.jhazmat.2005.11.015

[26] Wei, Y.-T., Wu, S.-C., Chou, C.-M., Che, C.-H., Tsai, S.-M., and Lien, H.-L., 2010, Influence of nanoscale zero-valent iron on geochemical properties of groundwater and vinyl chloride degradation: A field case study, Water Res., 44(1), 131-140.10.1016/j.watres.2009.09.012

[27] Yu, R.-F., Chi, F.-H., Cheng, W.-P., and Chang, J.-C., 2014, Application of pH, ORP, and DO monitoring to evaluate chromium(VI) removal from wastewater by the nanoscale zero-valent iron (nZVI) process, Chem. Eng. J., 255, 568-576.10.1016/j.cej.2014.06.002

[28] Zhang, W.-X. and Elliott, D.W., 2006, Applications of iron nanoparticles for groundwater remediation, Remediati. J., 16(2), 7-21.10.1002/rem.20078

Journal of Soil and Groundwater Environment ISSN:1598-6438(Print) 2287-8831(Online) 지하수토양환경

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