TECHNICAL PAPERS
Aug 15, 2003

Plasma-Assisted Process for Removing NO/NOx from Gas Streams with C2H4 as Additive

Publication: Journal of Environmental Engineering
Volume 129, Issue 9

Abstract

NOx removal from gas streams via dielectric barrier discharges (DBDs) has been experimentally evaluated. This paper investigates the effect of injecting C2H4 as an additive with respect to the De-NOx chemistry and the effect of gas composition on NO/NOx removal efficiencies. Experimental results indicate that both removal efficiencies of NO and NOx are enhanced with increasing applied voltage, gas temperature, and water vapor. Water vapor in gas streams has a distinct influence on NOx removal by generating OH radicals to convert NO2 to form HNO3. NOx removal decreases with increasing oxygen content although NO removal increases with increasing oxygen content. As high as 100% of NO and 57% of NOx are removed at 140°C for the gas stream containing [NO]:[C2H4]:[H2O(g)]:[O2]:[N2]=0.05:0.2:3.0:5.0:91.75. Major mechanisms for NO and NOx removals in DBD processing with C2H4 as an additive are described in the text.

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References

Albritton, D. L.(1978). “Ion-neutral reaction-rate constants measured in flow reactors through 1977.” At. Data Nucl. Data Tables, 22, 1–101.
Atkinson, R., Baulch, D. L., Cox, R. A., Hampson, R. F., Jr., Kerr, J. A., Rossi, M. J., and Troe, J.(1997). “Evaluated kinetic and photochemical data for atmospheric chemistry: supplement VI. IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry.” J. Phys. Chem. Ref. Data, 26, 1329–1499.
Atkinson, R., Baulch, D. L., Cox, R. A., Hampson, R. F., Jr., Kerr, J. A., and Troe, J.(1992). “Evaluated kinetic and photochemical data for atmospheric chemistry: supplement IV. IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry.” J. Phys. Chem. Ref. Data, 21(6), 1125–1568.
Baulch, D. L., Cobos, C. J., Cox, R. A., Frank, P., Hayman, G., Just, T. H., Kerr, J. A., Murrells, T., Pilling, M. J., Troe, J., Walker, R. W., and Warnatz, J.(1994). “Evaluated kinetic data for combustion modelling. Supplement I.” J. Phys. Chem. Ref. Data, 23, 847–1033.
Bohn, B., and Zetzsch, C.(1998). “Formation of HO2 from OH and C2H2 in the presence of O2.J. Chem. Soc., Faraday Trans., 94, 1203–1210.
Brownsword, R. A., Hancock, G., and Heard, D. E.(1997). “Kinetics of the N+NCO reaction at 298 K.” J. Chem. Soc., Faraday Trans., 93, 2473–2475.
Chang, M. B., and Cheng, C. F.(1997a). “Low temperature SNCR process for NOx control.” Sci. Total Environ., 198, 73–78.
Chang, M. B., and Cheng, C. F.(1997b). “Plasma-assisted removal of NO from gas streams via ammonia injection.” Environ. Eng. Sci., 14, 193–200.
Chang, M. B., Kushner, M. J., and Rood, M. J.(1992). “Gas phase removal of NO from gas streams via dielectric barrier discharges.” Environ. Sci. Technol., 26, 777–781.
Cooper, W. F., Park, J., and Hershberger, J. F.(1993). “Product channel dynamics of the NCO+NO reaction.” J. Phys. Chem., 97, 3283–3290.
Cox, R. A., and Derwent, R. G.(1975). “Kinetics of the reaction of HO2 with nitric oxide and nitrogen dioxide.” J. Photochem., 4, 139.
Cox, R. A., and Tyndall, G. S.(1980). “Rate constants for the reactions of CH3O2 with HO2, NO and NO2 using molecular modulation spectrometry.” J. Chem. Soc., Faraday Trans. 2, 76, 153.
DeMore, W. B., Sander, S. P., Golden, D. M., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E., and Molina, M. J. (1997). Chemical kinetics and photochemical data for use in stratospheric modeling. Evaluation No. 12 JPL Publication, 97-4, 1–266.
Eliasson, B., and Kogelschatz, U. (1986). “Basic data for modeling of electrical discharges in gases oxygen.” Rep. No. KLR 86-11C, Brown Boveri Konzernforschung, CH-5405 Baden.
Endo, Y., Tsuchiya, S., Yamada, C., Hirota, E., and Koda, S.(1986). “Microwave kinetic spectroscopy of reaction intermediates: O+ethylene reaction at low pressure.” J. Chem. Phys., 85, 4446–4452.
Fan, W. Y., Knewstubb, P. F., Kaning, M., Mechold, L., Ropcke, J., and Davies, P. B.(1999). “A diode laser and modeling study of mixed (CH4-H2-O2) ac plasmas.” J. Phys. Chem. A, 103, 4118.
Fulle, D., Hamann, H. F., Hippler, H., and Jansch, C. P.(1997). “The high pressure range of the addition of OH to C2H2 and C2H4.Ber. Bunsenges. Phys. Chem., 101, 1433–1422.
Fulle, D., Hamann, H. F., Hippler, H., and Troe, J.(1998). “Temperature and pressure dependence of the addition reactions of HO to NO and to NO2. IV. Saturated laser-induced fluorescence measurements up to 1400 bar.” J. Chem. Phys., 108, 5391–5397.
Gentile, A. C. (1995). “Kinetic processes and plasma remediation of toxic gases.” PhD dissertation, University of Illinois at Urbana-Champaign.
Glaenzer, K., and Troe, J.(1974). “Reactions of alkyl radicals in the shock wave-induced pyrolysis of nitroalkanes.” Ber. Bunsenges. Phys. Chem., 78, 182.
Hayashi, M. (1985). “Electron collision cross sections for molecules determined from beam and swarm data.” Proc., Meeting of the 45th Int. Swarm Seminar and the Inelastic Electron-Molecular Collision Symp., Tahoe City, Calif., July 19–23.
Herron, J. T. (1999). “Evaluated chemical kinetic data for reactions of N(2D), N(2P), and N2(A3u+) in the gas phase.” J. Phys. Chem. Ref. Data, 28, 1453–1483.
Higashi, M., Uchida, S., Suzuki, N., and Fujii, K.(1992). “Soot elimination and NOx and SOx reduction in diesel-engine exhaust by a combination of discharge plasma and oil dynamics.” IEEE Trans. Plasma Sci., 20(1), 1.
Itikawa, Y., Hayashi, M., Ichimura, A., Onda, K., Sakimoto, K., Takayanagi, K., Nakamura, M., Nishimura, H., and Takayanagi, T.(1986). “Cross sections for collisions of electrons and photons with nitrogen molecules.” J. Phys. Chem. Ref. Data, 15(3), 985.
Knyazev, V. D., Bencsura, A., Stoliarov, S. I., and Slagle, I. R.(1996). “Kinetics of the C2H3+H2=H+C2H4 and CH3+H2=H+CH4 reactions.” J. Phys. Chem., 100, 11346–1135.
Konnov, A. A. (2000). “Development and validation of a detailed reaction mechanism for the combustion of small hydrocarbons.” Proc., 28th Int. Symp. on Combustion, Edinburgh, U.K., p. 317.
Lee, C., Graves, D. B., Lieberman, M. A., and Hess, D. W.(1994). “Global-model of plasma chemistry in a high-density oxygen discharge.” J. Electrochem. Soc., 141(6), 1546.
Lee, S. Y., Yoo, H. S., Kang, W. K., and Jung, K. H.(1996). “Reaction of O(3P) atoms with CF2=Cxy (x,y=H,F,Cl,Br). Discharge flow-chemiluminescence imaging technique.” Chem. Phys. Lett., 257, 415–420.
Li, X., Sayah, N., and Jackson, W. M.(1985). “A large vibrational enhancement in the reaction of CN(v=1,2)+NO.J. Chem. Phys., 83, 616.
Lin, M. C., He, Y., and Melius, C. F.(1993). “Theoretical aspects of product formation from the NCO+NO reaction.” J. Phys. Chem., 97, 9124–9128.
Mahmud, K., Marshall, P., and Fontijn, A.(1987). “A high-temperature photochemistry kinetics study of the reaction of O(3P) atoms with ethylene from 290 to 1510 K.” J. Phys. Chem., 91, 1568.
Miller, J. A., and Bowman, C. T.(1989). “Mechanism and modeling of nitrogen chemistry in combustion.” Prog. Energy Combust. Sci., 15, 287.
Mizuno, A., Chakrabarti, A., and Okazaki, K. (1993). “Application of corona technology in the reduction of greenhouse gases and other gaseous pollutants.” Nonthermal plasma techniques for pollution control, B. M. Penetrante, Ed., 1993, Part B, Springer-Verlag, New York, 165–186.
Mizuno, A., Shimizu, K., Chakrabarti, A., Dascalescu, L., and Furuta, S.(1995). “NOx removal process using pulsed discharge plasma.” IEEE Trans. Ind. Appl., 31(5), 957–963.
Mizuno, A., Shimizu, K., Yanagihara, K., Kinoshita, K., Tsunoda, H., Kim, H., and Katsura, S.(1996). “Effect of additives and catalysts on removal of nitrogen oxides using pulsed discharge.” Conf. Rec. IEEE-IAS Annu. Meeting, Vol. 3, San Diego, Oct. 6–10, 1808–1812.
Nguyen, M. T., Sengupta, D., and Vanquickenborne, L. G.(1996). “Kinetic analyses combining quantum chemical and quantum statistical methods: some case studies.” J. Phys. Chem., 100, 10956–1096.
Niessen, W., Wolf, O., Schruft, R., and Neiger, M.(1998). “The influence of ethene on the conversion of NOx in a dielectric barrier discharge.” J. Phys. D, 31(5), 542–550.
NIST. (2000). “NIST Standard Reference Database No. 69.” February 2000 release.
Oda, T., Kato, T., Takahashi, T., and Shimizu, K.(1996a). “Nitric oxide decomposition in air by using nonthermal plasma processing—with additives and catalyst.” Conf. Rec. IEEE-IAS Annu. Meeting, Vol. 3, San Diego, Oct. 6–10, 1803–1807.
Oda, T., Kato, T., Takahashi, T., and Shimizu, K. (1996b). “Nitric oxide decomposition in air by using nonthermal plasma processing.” Proc., IEJ-ESA 1996 Joint Symp. Electrostatics, Univ. of Tokyo, Oct. 30–31, 17–28.
Okada, S., Tezaki, A., Miyoshi, A., and Matsui, H.(1994). “Product branching fractions in the reactions of NH and NH3 with NO.” J. Chem. Phys., 101, 9582–9588.
Paraskevopoulos, G., Preston, K. F., and Cvetanovic, R. J.(1971). “Relative rate of deactivation of O(1D) by molecular oxygen.” J. Chem. Phys., 54, 3907.
Park, J., and Hershberger, J. F.(1993a). “Kinetics and product branching ratios of the CN+NO2 reaction.” J. Chem. Phys., 99, 3488.
Park, J., and Hershberger, J. F.(1993b). “A diode laser study of the NCO+NO2 reaction.” J. Phys. Chem., 97, 13647.
Park, J., and Lin, M. C.(1997a). “Laser-initiated NO reduction by NH3: total rate constant and product branching ratio measurements for the NH2+NO reaction.” J. Phys. Chem. A, 101, 5–13.
Park, J., and Lin, M. C.(1997b). “A mass spectrometric study of the NH2+NO2 reaction.” J. Phys. Chem. A, 101, 2643.
Penetrante, B. M. (1993). “Plasma chemistry and power consumption in DeNOx.Nonthermal plasma techniques for pollution control, B. M. Penetrante, ed., Part A, Springer-Verlag, New York, 65–89.
Penetrante, B. M., Brusasco, R. M., Merritt, B. T., Pitz, W. J., and Vogtlin, G. E. (1999). “Feasibility of plasma aftertreatment for simultaneous control of NOx and particulates.” SAE paper 1999-01-3637.
Person, J. C., and Ham, D. O.(1988). “Removal of SO2 and NOx from stack gases by electron-beam irradiation.” Radiat. Phys. Chem., 31, 1.
Phelps, A. V. (1985). “Tabulations of collision cross sections and calculated transport and reaction coefficients for electron collisions with O2.JILA Information Center Rep. No. 28, Univ. of Colorado, Boulder, Colo.
Pruss, Jr., F. J., Slagle, I. R., and Gutman, D.(1974). “Determination of branching ratios for the reaction of oxygen atoms with ethylene.” J. Phys. Chem., 78, 663.
Quandt, R. W., and Hershberger, J. F.(1995). “Product branching ratios of the NH+NO and NH+NO2 reactions.” J. Phys. Chem., 99, 16939.
Smalley, J. F., Klemm, R. B., and Nesbitt, F. L. (1986). “Branching ratio for the hydrogen atom product channel in the reaction of ground-state atomic oxygen with ethylene.” J. Phys. Chem., 90, 491–497.
Smyth, K. C.(1996). “NO production and destruction in a methane/air diffusion flame.” Combust. Sci. Technol., 115, 151.
Sridharan, U. C., and Kaufman, F.(1983). “Primary products of the O+C2H4 reaction.” Chem. Phys. Lett., 102, 45.
Tsang, W., and Hampson, R. F.(1986). “Chemical kinetic data base for combustion chemistry. Part I. Methane and related compounds.” J. Phys. Chem. Ref. Data, 15, 1087.
Tsang, W., and Herron, J. T.(1991). “Chemical kinetic data base for propellant combustion. I. Reactions involving NO, NO2, HNO, HNO2, HCN and N2O.J. Phys. Chem. Ref. Data, 20, 609–663.
Vogtlin, G. E., and Penetrante, B. E. (1993). “Pulsed corona discharge for removal of NO from flue gas.” Nonthermal plasma techniques for pollution control, B. M. Penetrante, ed., Springer-Verlag, New York, 187–198.
Westenberg, A. A., and DeHaas, N.(1969). “Absolute measurements of the O+C2H4 rate coefficient.” Symp. Int. Combust. Proc., 12, 289.
Yamamoto, T., Yang, C. L., Kravets, Z., and Beltran, M.(2000). “Plasma assisted chemical reactor for NO decomposition.” IEEE Trans. Ind. Appl., 36, 923–927.

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Go to Journal of Environmental Engineering
Journal of Environmental Engineering
Volume 129Issue 9September 2003
Pages: 800 - 810

History

Received: Aug 29, 2000
Accepted: Nov 19, 2002
Published online: Aug 15, 2003
Published in print: Sep 2003

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How Ming Lee
PhD, Graduate Institute of Environmental Engineering, National Central Univ., Chungli, Taiwan 320, Republic of China.
Moo Been Chang
Professor, Graduate Institute of Environmental Engineering, National Central Univ., Chungli, Taiwan 320, Republic of China.
Shyh Chaur Yang
MS, Graduate Institute of Environmental Engineering, National Central Univ., Chungli, Taiwan 320, Republic of China.

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