Computer-simulated degradation of CF3Cl, CF2Cl2, and CFCl3 under electron beam irradiation

Kabasa, Stephen; Sun, Yongxia; Chmielewski, Andrzej G.; Nichipor, Henrietta

doi:10.2478/nuka-2023-0009

Abstract

Electron beam treatment technologies should be versatile in the removal of chlorofluorocarbons (CFCs) owing to their exceptional cross sections for the thermal electrons generated in the radiolysis of air. Humidity, dose rates, O₂ concentration, and CFC concentration influence the efficiency of the destruction process under electron beam treatment. Computer simulations have been used to theoretically demonstrate the destruction of chlorotrifluoromethane (CF₃Cl), dichlorodifluoromethane (CF₂Cl₂), and trichlorofluoromethane (CFCl₃) in the air (N₂ + O₂: 80% + 20%) in room temperature up to a dose of 13 kGy. Under these conditions, it is predicted that the removal efficiency is in the order CF₃Cl (0.1%) < CF₂Cl₂ (7%) < CFCl₃ (34%), which shows the dependence of the process on the number of substituted Cl atoms. Dissociative electron attachment with the release of Cl^– is the primary process initiating the destruction of CFCs from the air stream. Reactions with the first excited state of oxygen, namely, O(¹D), and charge-transfer reactions further promote the degradation process. The degradation products can be further degraded to CO₂, Cl₂, and F₂ by prolonged radiation treatment. Other predicted products can also be removed through chemical processes.

References

Xiao, G., Xu, W., Wu, R., Ni, M., Du, C., Gao, X., Luo, Z., & Cen, K. (2014). Non-thermal plasmas for VOCs abatement. Plasma Chem. Plasma Process., 34(5), 1033–1065. https://doi.org/10.1007/s11090- 014-9562-0.
Search in Google Scholar Back to article
Chmielewski, A. G. (1995). Electron beam gaseous pollutants treatment. In International Conference on Plasma Science, 5–8 June 1995, Madison, WI, USA (p. 269). DOI: 10.1109/PLASMA.1995.533498.
Open DOI Search in Google Scholar Back to article
Denifl, G., Muigg, D., Walker, I., Cicman, P. T., Matejcik, S., Skalny, J. D., Stamatovic, A., & Märk, T. D. (1999). Dissociative electron attachment to CF2Cl2. Czech. J. Phys., 49(3), 383–392. https://doi.org/10.1023/A:1022857202672.
Search in Google Scholar Back to article
Wang, Y. F., Lee, W. J., Chen, C. Y., Wu, Y. P. G., & Chang-Chien, G. P. (2000). Reaction mechanisms in both a CCl2F2/O2/Ar and a CCl2F2/H2/Ar RF plasma environment. Plasma Chem. Plasma Process., 20(4), 469–494. https://doi.org/10.1023/A:1007027805680.
Search in Google Scholar Back to article
Stoiber, T., Evans, S., & Naidenko, O. V. (2020). Disposal of products and materials containing per- and polyfluoroalkyl substances (PFAS): A cyclical problem. Chemosphere, 260, 127659. https://doi.org/10.1016/j.chemosphere.2020.127659.
Search in Google Scholar Back to article
Ross, I., McDonough, J., Miles, J., Storch, P., Thelak- kat Kochunarayanan, P., Kalve, E., Hurst, J., Das- gupta, S., & Burdick, J. (2018). A review of emerging technologies for remediation of PFASs. Remediation, 28(2), 101–126. https://doi.org/10.1002/rem.21553.
Search in Google Scholar Back to article
Dahiru, U. H., Saleem, F., Zhang, K., & Harvey, A. P. (2021). Removal of cyclohexane as a toxic pollutant from air using a non-thermal plasma: Influence of different parameters. J. En iron. Chem. Eng., 9(1), 105023. https://doi.org/10.1016/j.jece.2021.105023.
Search in Google Scholar Back to article
Hakoda, T., Hashimoto, S., & Kojima, T. (2002). Ef- fect of water and oxygen contents on the decomposi- tion of gaseous trichloroethylene in air under electron beam irradiation. Bull. Chem. Soc. Jpn., 75(10). https://doi.org/10.1246/bcsj.75.2177.
Search in Google Scholar Back to article
Hirota, K., Hakoda, T., Arai, H., & Hashimoto, S. (2002). Electron-beam decomposition of vaporized VOCs in air. Radiat. Phys. Chem., 65(4/5), 415–421. https://doi.org/10.1016/S0969-806X(02)00353-5.
Search in Google Scholar Back to article
Kim, H. H., Prieto, G., Takashima, K., Katsura, S., & Mizuno, A. (2002). Performance evaluation of dis- charge plasma process for gaseous pollutant removal. J. Electrost., 55(1), 25–41. https://doi.org/10.1016/S0304-3886(01)00182-6.
Search in Google Scholar Back to article
Dobslaw, C., & Glocker, B. (2020). Plasma tech- nology and its relevance in waste air and waste gas treatment. Sustainability, 12(21), 1–39. https://doi.org/10.3390/su12218981.
Search in Google Scholar Back to article
Cooper, R., & Mezyk, S. P. (2001). Fundamental processes in gas phase radiation chemistry. Studies in Physical and Theoretical Chemistry C, 87, 107–144. https://doi.org/10.1016/S0167-6881(01)80008-2.
Search in Google Scholar Back to article
Chmielewski, A. G., Sun, Y., Licki, J., Pawelec, A., Wit- man, S., & Zimek, Z. (2012). Electron beam treatment of high NOx concentration off-gases. Radiat. Phys. Chem., 81(8), 1036–1039. https://doi.org/10.1016/j.radphyschem.2011.12.012.
Search in Google Scholar Back to article
Kashiwagi, M., & Hoshi, Y. (2012). Electron beam processing system and its application. SEI Tech. Re ., 75, 47–54.
Search in Google Scholar Back to article
Gogulancea, V., & Lavric, V. (2014). Flue gas cleaning by high energy electron beam – modeling and sensitivity analysis. Appl. Therm. Eng., 70(2), 1253–1261. https://doi.org/10.1016/j.applthermaleng.2014.05.046.
Search in Google Scholar Back to article
Illenberger, E. (1992). Electron-attachment reactions in molecular clusters. Chem. Re ., 92(7), 1589–1609. https://doi.org/10.1021/cr00015a006.
Search in Google Scholar Back to article
Jones, R. K. (1984). Absolute total cross section for the scattering of low energy electrons by methane. J. Chem. Phys., 82(12), 5424–5427. https://doi.org/10.1063/1.448575.
Search in Google Scholar Back to article
Won, Y. S., Han, D. H., Stuchinskaya, T., Park, W. S., & Lee, H. S. (2002). Electron beam treatment of chloroethylenes/air mixture in a flow reactor. Radiat. Phys. Chem., 63(2), 165–175. https://doi.org/10.1016/S0969-806X(01)00237-7.
Search in Google Scholar Back to article
Kim, J., Han, B., Kim, Y., Lee, J. H., Park, C. R., Kim, J. C., Kim, J. C., & Kim, K. J. (2004). Removal of VOCs by hybrid electron beam reactor with catalyst bed. Radiat. Phys. Chem., 71(1/2), 429–432. https://doi.org/10.1016/J.RADPHYSCHEM.2004.04.015.
Search in Google Scholar Back to article
Han, D. H., Stuchinskaya, T., Won, Y. S., Park, W. S., & Lim, J. K. (2003). Oxidative decomposition of aromatic hydrocarbons by electron beam irradia- tion. Radiat. Phys. Chem., 67(1), 51–60. https://doi.org/10.1016/S0969-806X(02)00405-X.
Search in Google Scholar Back to article
Nichipor, H., Yacko, S., Sun, Y., Chmielewski, A. G., & Zimek, Z. (2008). Theoretical study of dose and dose rate effect on trichloroethylene (HClC=CCl2) decomposition in dry and humid air under electron beam irradiation. Nukleonika, 53(1), 11–16.
Search in Google Scholar Back to article
Fabian, P., & Borchers, R. (2001). Growth of halo- carbon abundances in the stratosphere between 1977 and 1999. Ad?. Space Res., 28(7), 961–964. https://doi.org/10.1016/S0273-1177(01)80024-7.
Search in Google Scholar Back to article
Midgley, P. M., & McCulloch, A. (1999). Production, sales and emissions of halocarbons from industrial sources. In P. Fabian & O. N. Singh (Eds.). Reac- ti e halogen compounds in the atmosphere. (The Handbook of Environmental Chemistry, Vol. 4E, pp. 155–190). Berlin, Heidelberg: Springer. https://doi.org/10.1007/10628761_6.
Search in Google Scholar Back to article
Foglein, K. A., Szépvölgyi, J., Szabó, P. T., Mészáros, E., Pekker-Jakab, E., Babievskaya, I. Z., Mohai, I., & Károly, Z. (2005). Comparative study on decompo- sition of CFCl3 in thermal and cold plasma. Plasma Chem. Plasma Process., 25(3), 275–288. https://doi.org/10.1007/s11090-004-3040-z.
Search in Google Scholar Back to article
Yokoi, A., Kuchar, D., Kubota, M., Liwei, H., Ushi- roebisu, K., & Matsuda, H. (2008). Comparison of non-thermal plasma decomposition characteristics of organo-halide gases under oxidizing and reducing atmosphere. Global NEST Journal, 10(2), 249–254.
Search in Google Scholar Back to article
Codnia, J., & Azcárate, M. L. (2006). Rate mea- surement of the reaction of CF2Cl radicals with O2. Photochem. Photobiol., 82(3), 755. https://doi.org/10.1562/2006-01-04-ra-764.
Search in Google Scholar Back to article
Xavier, E. S., Rocha, W. R., Da Silva, J. C. S., Dos Santos, H. F., & De Almeida, W. B. (2007). Ab initio thermodynamic study of the reaction of CF2Cl2 and CHF2Cl CFCs species with OH radical. Chem. Phys. Lett., 448(4/6), 164–172. https://doi.org/10.1016/j.cplett.2007.09.086.
Search in Google Scholar Back to article
Faradzhev, N. S., Perry, C. C., Kusmierek, D. O., Fairbrother, D. H., & Madey, T. E. (2004). Kinetics of electron-induced decomposition of CF2Cl2 coad- sorbed with water (ice): A comparison with CCl4. J. Chem. Phys., 121(17), 8547–8561. https://doi.org/10.1063/1.1796551.
Search in Google Scholar Back to article
Lengyel, J., van der Linde, C., Fárník, M., & Beyer, M. K. (2016). The reaction of CF2Cl2 with gas-phase hydrated electrons. Phys. Chem. Chem. Phys., 18(34), 23910–23915. https://doi.org/10.1039/c6cp01976e.
Search in Google Scholar Back to article
Nakayama, N., Wilson, S. C., Stadelmann, L. E., Lee, H. L. D., Cable, C. A., & Arumainayagam, C. R. (2004). Low-energy electron-induced chemis- try of CF2Cl2: Implications for the ozone hole? J. Phys. Chem. B, 108(23), 7950–7954. https://doi.org/10.1021/jp031319j.
Search in Google Scholar Back to article
Anshumali, Winkleman, B. C., & Sheth, A. (1997). Destruction of low levels of volatile organic com- pounds in dry air streams by an electron-beam gen- erated plasma. J. Air Waste Manage. Assoc., 47(12), 1276–1283. https://doi.org/10.1080/10473289.199 7.10464071.
Search in Google Scholar Back to article
Yamamoto, T., & Futamura, S. (1998). Nonthermal plasma processing for controlling volatile organic com- pounds. Combust. Sci. Technol., 133(1/3), 117–133. https://doi.org/10.1080/00102209808952031.
Search in Google Scholar Back to article
Nichipor, H., Dashouk, E., Chmielewski, A. G., Zimek, Z., & Bulka, S. (2000). A theoretical study on decomposition of carbon tetrachloride, trichlo- roethylene and ethyl chloride in dry air under the influence of an electron beam. Radiat. Phys. Chem., 57(3/6), 519–525. https://doi.org/10.1016/S0969- 806X(99)00454-5.
Search in Google Scholar Back to article
Burns, S. J., Matthews, J. M., & McFadden, D. L. (1996). Rate coefficients for dissociative electron at- tachment by halomethane compounds between 300 and 800 K. J. Phys. Chem., 100(50), 19436–19440. https://doi.org/10.1021/jp962529h.
Search in Google Scholar Back to article
Illenberger, E., Scheunemann, H. U., & Baumgär- tel, H. (1979). Negative ion formation in CF2Cl2, CF3Cl and CFCl3 following low energy (0–10 eV) impact with near monoenergetic electrons. Chem. Phys., 37(1), 21–31. https://doi.org/10.1016/0301- 0104(79)80003-8.
Search in Google Scholar Back to article
Klar, D., Ruf, M. W., & Hotop, H. (2001). Dissociative electron attachment to CCl4 molecules at low electron energies with meV resolution. Int. J. Mass Spectrom., 205(1/3), 93–110. https://doi.org/10.1016/S1387- 3806(00)00271-2.
Search in Google Scholar Back to article
Durbin, D. E., Wentworth, W. E., & Zlatkis, A. (1970). Reactions between electron absorbing organic compounds and electrons at near thermal energies. J. Am. Chem. Soc., 92(17), 5131–5136. https://doi.org/10.1021/ja00720a023.
Search in Google Scholar Back to article
Gal, A., Ogata, A., Futamura, S., & Mizuno, K. (2003). Mechanism of the dissociation of chloro- fluorocarbons during nonthermal plasma processing in nitrogen at atmospheric pressure. J. Phys. Chem. A, 107(42), 8859–8866. https://doi.org/10.1021/jp0347769.
Search in Google Scholar Back to article
Miller, T. M. (2005). Thermal electron attachment and detachment in gases. Ad ances in Atomic, Molecular and Optical Physics, 51(5), 299–342. https://doi.org/10.1016/S1049-250X(05)51018-8.
Search in Google Scholar Back to article
Atkinson, R., Hansen, D. A., & Pitts, J. N. (1975). Rate constants for the reaction of OH radicals with CHF2Cl, CF2Cl2, CFCl3, and H2 over the temperature range 297-434 K. J. Chem. Phys., 63(5), 1703. https://doi.org/10.1063/1.431566.
Search in Google Scholar Back to article
DeMore, W. B., & Bayes, K. D. (1999). Rate con- stants for the reactions of hydroxyl radical with several alkanes, cycloalkanes, and dimethyl ether. J. Phys. Chem. A, 103(15), 2649–2654. https://doi.org/10.1021/jp983273d.
Search in Google Scholar Back to article
Graupner, K., Haughey, S. A., Field, T. A., Mayhew, C. A., Hoffmann, T. H., May, O., Fedor, J., Allan, M., Fabrikant, I. I., Illenberger, E., Braun, M., Ruf, M. W., & Hotop, H. (2010). Low-energy electron attachment to the dichlorodifluoromethane (CCl2F2) molecule. J. Phys. Chem. A, 114(3), 1474–1484. https://doi.org/10.1021/jp9081992.
Search in Google Scholar Back to article
Willis, C., Boyd, A. W., Young, M. J., & Armstrong, D. A. (1970). Radiation chemistry of gaseous oxygen: experimental and calculated yields. Can. J. Chem., 48(10), 246. https://doi.org/10.1139/v70-246.
Search in Google Scholar Back to article
Atkinson, R., Connell, P. S., Dorn, H. P., Derudder, A., & Isaksen, I. S. (1990). Halocarbon ozone depletion and global warming potentials N92-15434. In R. A. Cox & D. Wuebbles (Eds.), Scientific assessment of stratospheric ozone (Vol. 4, pp. 4.1-4.192). Scientific Assessment of Stratospheric Ozone.
Search in Google Scholar Back to article
Harrison, J. J., Chipperfield, M. P., Dudhia, A., Cai, S., Dhomse, S., Boone, C. D., & Bernath, P. F. (2014). Satellite observations of stratospheric carbonyl fluoride. Atmos. Chem. Phys., 14(21), 11915–11933. https://doi.org/10.5194/acp-14-11915-2014.
Search in Google Scholar Back to article
Hayman, G. D., Solomon, S., Howard, C., Kanakidou, M., & Penkett, S. A. (1994). Atmospheric degradation of halocarbon substitutes. Scientific Assessment of Ozone Depletion, 37, 12.1-12.17.
Search in Google Scholar Back to article
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., & Wallington, T. J. (2008). Evaluated kinetic and photochemical data for atmo- spheric chemistry: Volume IV – Gas phase reactions of organic\newline halogen species. Atmos. Chem. Phys., 8(15), 4141–4496. https://doi.org/10.5194/acp-8-4141-2008.
Search in Google Scholar Back to article
Burkholder, J. B., Cox, R. A., & Ravishankara, A. R. (2015). Atmospheric degradation of ozone deplet- ing substances, their substitutes, and related spe- cies. Chem. Re ., 115(10), 3704–3759. https://doi.org/10.1021/cr5006759.
Search in Google Scholar Back to article
Cox, R. A., Ammann, M., Crowley, J. N., Herrmann, H., Jenkin, M. E., McNeill, F. V., Wahid Mellouki, A., Rossi, M. J., Troe, J., & Wallington, T. J. (2019, April 22). IUPAC in the (real) clouds. International Union of Pure and Applied Chemistry. https://iupac.org/100/stories/iupac-in-the-clouds/.
Search in Google Scholar Back to article
Jeon, E. C., Kim, K. J., Kim, J. C., Kim, K. H., Chung, S. G., Sunwoo, Y., & Park, Y. K. (2008). Novel hybrid technology for VOC control using an electron beam and catalyst. Res. Chem. Intermediat., 34(8/9), 863–870. https://doi.org/10.1007/BF03036948.
Search in Google Scholar Back to article
Son, Y. S., Kim, K. J., & Kim, J. C. (2010). A review on VOCs control technology using electron beam. Asian J. Atmos. En iron., 4(2), 63–71. https://doi.org/10.5572/ajae.2010.4.2.063.
Search in Google Scholar Back to article
Sun, Y., Chmielewski, A. G., Licki, J., Bulka, S., & Zimek, Z. (2009). Decomposition of organic compounds in simulated industrial off-gas by using electron beam irradiation. Radiat. Phys. Chem., 78(7/8), 721–723. https://doi.org/10.1016/j.radphy-schem.2009.03.049.
Search in Google Scholar Back to article
Han, D. -H. H., Stuchinskaya, T., Won, Y. -S. S., Park, W. -S. S., & Lim, J. -K. K. (2003). Oxidative decomposition of aromatic hydrocarbons by electron beam irradiation. Radiat. Phys. Chem., 67(1), 51–60. https://doi.org/10.1016/s0969-806x(02)00405-x.
Search in Google Scholar Back to article
Hirota, K., Sakai, H., Washio, M., & Kojima, T. (2004). Application of electron beams for the treat- ment of VOC streams. Ind. Eng. Chem. Res., 43(5), 1185–1191. https://doi.org/10.1021/ie0340746.
Search in Google Scholar Back to article
Sun, Y. X., Hakoda, T., Chmielewski, A. G., & Hashi- moto, S. (2003). Trans-1,2-dichloroethylene decom- position in low-humidity air under electron beam irradiation. Radiat. Phys. Chem., 68(5), 843–850. https://doi.org/10.1016/S0969-806X(03)00347-5.
Search in Google Scholar Back to article
Sun, Y. X., Hakoda, T., Chmielewski, A. G., Hashi- moto, S., Zimek, Z., Bulka, S., Ostapczuk, A., & Nichipor, H. (2001). Mechanism of 1,1-dichloroethyl- ene decomposition in humid air under electron beam irradiation. Radiat. Phys. Chem., 62(4), 353–360. https://doi.org/10.1016/S0969-806X(01)00200-6.
Search in Google Scholar Back to article
Penetrante, B. M., Hsiao, M. C., Bardsley, J. N., Mer- ritt, B. T., Vogtlin, G. E., Kuthi, A., Burkhart, C. P., & Bayless, J. R. (1997). Identification of mechanisms for decomposition of air pollutants by non-thermal plas- ma processing. Plasma Sources Sci. Technol., 6(3), 251. https://doi.org/10.1088/0963-0252/6/3/002.
Search in Google Scholar Back to article
Aleksandrov, N. L., & Bazelyan, E. M. (1999). Ionization processes in spark discharge plasmas. Plasma Sources Sci. Technol., 8(2), 285. https://doi.org/10.1088/0963-0252/8/2/309.
Search in Google Scholar Back to article
Lietz, A. M., & Kushner, M. J. (2018). Molecular admixtures and impurities in atmospheric pressure plasma jets. J. Appl. Phys., 124(15), 153303. https://doi.org/10.1063/1.5049430.
Search in Google Scholar Back to article
Chmielewski, A. G., Sun, Y., Bulka, S., & Zimek, Z. (2007). Review on gaseous chlorinated organic pollut- ants electron beam treatment. Radiat. Phys. Chem., 76(11/12), 1795–1801. https://doi.org/10.1016/j.radphyschem.2007.02.102.
Search in Google Scholar Back to article
Sun, Y., Chmielewski, A. G., Bulka, S., & Zimek, Z. (2007). 1-Chloronaphthalene decomposition in dif- ferent gas mixtures under electron beam irradiation. Radiat. Phys. Chem., 76(11/12), 1802–1805. https://doi.org/10.1016/j.radphyschem.2007.02.111.
Search in Google Scholar Back to article

Computer-simulated degradation of CF3Cl, CF2Cl2, and CFCl3 under electron beam irradiation

Abstract

Paradigm

My account