Benzene degradation in waste gas by photolysis and photolysis-ozonation: experiments and modeling
Fariba Mahmoudkhani, Maryam Rezaei, Vahid Asili, Mahsasadat Atyabi, Elena Vaisman, Cooper H. Langford, Alex De Visscher
Benzene degradation in waste gas by photolysis and photolysis-ozonation: experiments and modeling
A photochemical model of benzene degradation compares well with experimental data obtained in the Lab.
62 reactions were needed to fully describe benzene degradation.
A feasibility study shows that the photolysis of benzene is a cost-effective process.
Experimental data and modeling results show that the degradation efficiency will increase when the combination of UV light and ozone is used.
The degradation of benzene, a carcinogenic air pollutant, was studied in a gas-phase photochemical reactor with an amalgam lamp emitting ultraviolet light at 185 and 254 nm. Efficient benzene degradation (>70%) was possible for benzene mass flow rates of up to 1.5 mg·min−1. Adding ozone allowed benzene mass flow rates of up to 5 mg·min−1 to be treated with the same efficiency. In terms of energy consumption, ozone doubles the efficiency of the process. A comprehensive mechanistic simulation model was developed incorporating a chemical kinetics model (62 reactions involving 47 chemical species), a material balance model incorporating diffusion and flow, a flow velocity model, and a light field model. The model successfully predicted the efficiency of the reactor, generally within 20%, which indicates that the model is sound, and can be used for feasibility studies. The prediction of the reactor efficiency in the presence of ozone was less successful, with systematically overestimated efficiency. Condensation of reaction products in the reactor is thought to be the main cause of model inaccuracy. Both experimental data and model predictions show that there is a synergistic effect between ozonation and ultraviolet degradation.
Photolysis / Ozone / Benzene / Waste gas / Simulation / Synergism
[1] |
Kamps R, Müller H, Schmitt M, Sommer S, Wang Z, Kleinermanns K. Photooxidation of exhaust pollutants: I. Degradation efficiencies, quantum yields and products of benzene photooxidation. Chemosphere, 1993, 27(11): 2127–2142
CrossRef
Google scholar
|
[2] |
Wang C, Xi J Y, Hu H Y, Xi J Y, Hu H Y, Arhami M, Polidori A, Polidori A, Delfino R, Tjoa T, Tjoa T, Sioutas C, Wang C, Xi J Y, Hu H Y, Xi J Y, Hu H Y, Pacheco A, Freitas M, Pratt G, Dymond M, Dymond M, Krzyzanowski J, Luo H L, Chang W C, Lin D F, Pennell K, Bozkurt O, Suuberg E, Bozkurt O, Suuberg E, Isakov V, Touma J, Burke J, Touma J, Burke J, Lobdell D, Palma T, Rosenbaum A, zkaynak H, Lipfert F, Wyzga R, Baty J, Miller J, Miller J, Mohan R, Leonardi G, Robins A, Jefferis S, Jefferis S, Coy J, Wight J, Wight J, Murray V. Effects of operation conditions on removal rate constant and quantum yield of gaseous chlorobenzene degradation in a photochemical reactor. Journal of the Air & Waste Management Association, 2009, 59(4): 386–391
CrossRef
Google scholar
|
[3] |
Zhang L, Anderson W A. Kinetic analysis of the photochemical decomposition of gas-phase chlorobenzene in a UV reactor: Quantum yield and photonic efficiency. Chemical Engineering Journal, 2013, 218(a): 247–252
|
[4] |
Zhang L, Anderson W A. Effect of ozone and sulfur dioxide on the photolytic degradation of chlorobenzene in air. Industrial and Engineering Chemistry Research, 2013, 52(b): 3315–3319
|
[5] |
Gürtler K R, Kleinermanns K. Photooxidation of exhaust pollutants: II. Photooxidation of chloromethanes: Degradation efficiencies, quantum yields and products. Chemosphere, 1994, 28(7): 1289–1298
CrossRef
Google scholar
|
[6] |
Chen F Y, Pehkonen S O, Ray M B. Kinetics and mechanisms of UV-photodegradation of chlorinated organics in the gas phase. Water Research, 2002, 36(17): 4203–4214
CrossRef
Google scholar
|
[7] |
Alapi T, Van Craeynest K, Van Langenhove H, Dombi A. UV photolysis of the binary mixtures of VOCs in dry nitrogen stream. Reaction Kinetics and Catalysis Letters, 2006, 87(2): 255–262
CrossRef
Google scholar
|
[8] |
Alapi T, Van Craeynest K, Van Langenhove H, Dewulf J, Dombi A. Direct VUV photolysis of chlorinated methanes and their mixtures in a nitrogen stream. Chemosphere, 2007, 66(1): 139–144
CrossRef
Google scholar
|
[9] |
Gürtler R, Möller U, Sommer S, Kleinermanns K. Photooxidation of exhaust pollutants: III. Photooxidation of the chloroethenes: Degradation efficiencies, quantum yields and products. Chemosphere, 1994, 29(8): 1671–1682
CrossRef
Google scholar
|
[10] |
Lee K Y, Lee J Y, Khinast J, Stencel J R, Lavid M. Photochemical remediation of tetrachloroethylene: Reactor design, construction, and preliminary results. Journal of Environmental Engineering, 2004, 130(1): 100–103
CrossRef
Google scholar
|
[11] |
Lee K Y, Lee J Y. Photochemical destruction of tetrachloroethylene and trichloroethylene from the exhaust of an air stripper. Journal of Environmental Engineering, 2005, 131(10): 1441–1446
CrossRef
Google scholar
|
[12] |
Chen J M, Cheng Z W, Jiang Y F, Zhang L L. Direct VUV photodegradation of gaseous a-pinene in a spiral quartz reactor: Intermediates, mechanism, and toxicity/biodegradability assessment. Chemosphere, 2010, 81(9): 1053–1060
CrossRef
Google scholar
|
[13] |
Cheng Z W, Jiang Y F, Zhang L L, Chen J M, Wei Y Y. Conversion characteristics and kinetic analysis of gaseous a-pinene degraded by VUV light in various reaction media. Separation and Purification Technology, 2011, 77(1): 26–32
CrossRef
Google scholar
|
[14] |
Shen Y S, Ku Y. Treatment of gas-phase volatile organic compounds (VOCs) by the UV/O3 process. Chemosphere, 1999, 38(8): 1855–1866
CrossRef
Google scholar
|
[15] |
Alapi T, Dombi A. Direct VUV photolysis of clorinated methanes and their mixtures in an oxygen stream using an ozone producing low-pressure mercury vapour lamp. Chemosphere, 2007, 67(4): 693–701
CrossRef
Google scholar
|
[16] |
Zuo G M, Cheng Z X, Chen H, Li G W, Miao T. Study on photocatalytic dagradation of several volatile organic compounds. Journal of Hazardous Materials, 2006, 128(2-3): 158–163
CrossRef
Google scholar
|
[17] |
Zhong J, Wang J, Tao L, Gong M, Zhimin L, Chen Y. Photocatalytic degradation of gaseous benzene over TiO2/Sr2CeO4: Kinetic model and degradation mechanisms. Journal of Hazardous Materials, 2007, B139(2): 323–331
CrossRef
Google scholar
|
[18] |
Krishnan J, Swaminathan T. Kinetic modeling of a photocatalytic reactor designed for removal of gas-phase benzene: A study on limiting resistances using design of experiments. Latin American Applied Research, 2010, 40: 359–364
|
[19] |
Bouzaza A, Vallet C, Laplanche A. Photocatalytic degradation of some VOCs in the gas phase using an annular flow reactor – Determination of the contribution of mass transfer and chemical reaction steps in the photodegradation process. Journal of Photochemistry and Photobiology A Chemistry, 2006, 177(2-3): 212–217
CrossRef
Google scholar
|
[20] |
Tomasic J F, Gomzi Z. Photocatalytic oxidation of toluene in the gas phase: Modelling an annular photocatalytic reactor. Catalysis Today, 2009, 137(2-4): 350–356
CrossRef
Google scholar
|
[21] |
Huang H. Removal of air pollutants by photocatalysis with ozone in a continuous-flow reactor. Environmental Engineering Science, 2010, 27(8): 651–656
CrossRef
Google scholar
|
[22] |
Shindo K, Lipsky S. Photochemistry of benzene vapor at 1849 Å. Journal of Chemical Physics, 1966, 45(6): 2292–2297
CrossRef
Google scholar
|
[23] |
Yokoyama A, Zhao X, Hintsa E J, Continetti R E, Lee Y T. Molecular beam studies of the photodissociation of benzene at 193 and 248 nm. Journal of Chemical Physics, 1990, 92(7): 4222–4233
CrossRef
Google scholar
|
[24] |
Calvert J C, Atkinson R, Becker K H, Kamens R M, Seinfeld J H, Wallington T J, Yarwood G. The Mechanisms of Atmospheric Oxidation of Aromatic Hydrocarbons. Oxford University Press, New York, 2002
|
[25] |
Chen F, Yang Q, Pehkonen S O, Ray M B. Modeling of gas-phase photodegradation of chloroform and carbon tetrachloride. Journal of the Air & Waste Management Association, 2004, 54(10): 1281–1292
CrossRef
Google scholar
|
[26] |
Asili V, De Visscher A. Mechanistic model for ultraviolet degradation of H2S and NOx in waste gas. Chemical Engineering Journal, 2014, 244: 597–603
CrossRef
Google scholar
|
[27] |
Kuo C H, Zhang L, Wang J, Zappi M E. Vapor and liquid phase ozonation of benzene. Ozone Science and Engineering, 1977, 19(2): 109–127
CrossRef
Google scholar
|
[28] |
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. Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I – Gas phase reactions of Ox, HOx, NOx and SOx species. Atmospheric Chemistry and Physics, 2004, 4: 1461–1738
CrossRef
Google scholar
|
[29] |
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, 0. Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – Gas phase reactions of organic species. Atmospheric Chemistry and Physics, 2006, 6(11): 3625–4055
CrossRef
Google scholar
|
[30] |
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. Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III – Gas phase reactions of inorganic halogens. Atmospheric Chemistry and Physics, 2007, 7(4): 981–1191
CrossRef
Google scholar
|
[31] |
Chen J, Davidson J H. Model of the negative DC corona plasma: Comparison to the positive DC corona plasma. Plasma Chemistry and Plasma Processing, 2003, 23(1): 83–102
CrossRef
Google scholar
|
[32] |
Orlando J J, Tyndall G S. The atmospheric chemistry of the HC(O)CO radical. International Journal of Chemical Kinetics, 2001, 33(3): 149–156
CrossRef
Google scholar
|
[33] |
Olariu R I I, Barnes I, Becker K H, Klotz B. Rate coefficients for the gas-phase reaction of OH radicals with selected dihydroxybenzenes and benzoquinones. International Journal of Chemical Kinetics, 2000, 32(11): 696–702
CrossRef
Google scholar
|
[34] |
Kwok E S C, Atkinson R. Estimation of hydroxyl radical reaction-rate constants for gas-phase organic-compounds using a structure-reactivity relationship – An update. Atmospheric Environment, 1995, 29(14): 1685–1695
CrossRef
Google scholar
|
[35] |
Brown A C, Canosas-Mas C E, Parr A D, Wayne R P. Temperature-dependence of the rate of the reaction between the OH radical and ketene. Chemical Physics Letters, 1989, 161(6): 491–496
CrossRef
Google scholar
|
[36] |
Sander S P, Friedl R R, Ravishankara A R, Golden D M, Kolb C E, Kurylo M S, Molina M J, Moortgat G K, Keller-Rudek H, Finlayson-Pitts B J, Wine P H, Huie R E, Orkin V L. Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies: Evaluation Number 15. JPL Publications, 2006, 06–2
|
[37] |
Volkamer R, Spietz P, Burrows J H U, Platt U. High-resolution absorption cross-section of glyoxal in the UV-vis and IR spectral ranges. Journal of Photochemistry and Photobiology A Chemistry, 2005, 172(1): 35–46
CrossRef
Google scholar
|
[38] |
Tang Y X, Zhu L. Photolysis of butenedial at 193, 248, 280, 308, 351, 400, and 450 nm. Chemical Physics Letters, 2005, 409(4-6): 151–156
CrossRef
Google scholar
|
[39] |
Yoshino K, Esmond J R, Cheung A S C, Freeman D E, Parkinson W H. High resolution absorption cross sections in the transmission window region of the Schumann-Runge bands and Herzberg continuum of O2. Planetary and Space Science, 1992, 40(2-3): 185–192
CrossRef
Google scholar
|
[40] |
Berndt T, Böge O. Formation of phenol and carbonyls from the atmospheric reaction of OH radicals with benzene. Physical Chemistry Chemical Physics, 2006, 8(10): 1205–1214
CrossRef
Google scholar
|
[41] |
Atkinson R J, Arey J. Atmospheric degradation of volatile organic compounds. Chemical Reviews, 2003, 103(12): 4605–4638
CrossRef
Google scholar
|
[42] |
Jenkin M E, Saunders S M, Wagner V, Pilling M J. Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part B): Tropospheric degradation of aromatic volatile organic compounds. Atmospheric Chemistry and Physics, 2003, 3(1): 181–193
CrossRef
Google scholar
|
[43] |
De Visscher A, Dewulf J, Van Durme J, Leys C, Morent R, Van Langenhove H. Non-thermal plasma destruction of allyl alcohol in waste gas: Kinetics and modelling. Plasma Sources Science & Technology, 2008, 17(1): 015004
CrossRef
Google scholar
|
[44] |
Bird R B, Steward W E, Lightfoot E N. Transport Phenomena, 2nd edition. New York: John Wiley & Sons, 2002
|
/
〈 | 〉 |