Experimental and Modeling Study on de-NOx Characteristics of Selective Non-catalytic Reduction in O2/CO2 Atmosphere

doi:10.1016/j.cjche.2014.06.002

摘要/Abstract

摘要： An experimental study of thermal de-NO_x using NH₃ as reductant in O₂/CO₂ atmosphere with the effect of SO₂ and different additiveswas performed in a drop tube furnace. Results show that the optimum temperature window is 841-1184℃, and the optimumreaction temperature is about 900℃ with a de-NO_x efficiency of 95.4%. A certain amount of SO₂ has an inhibiting effect on NO reduction. The effect of additives, including Na₂CO₃, C₂H₅OH and FeCl₃, on NO reduction by NH₃ is also explored. The addition of Na₂CO₃ and FeCl₃ is useful towiden the temperature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800℃. Qualitatively, the modeling results using a detailed kinetic modeling mechanism represent well most of the process features. The effect of Na₂CO₃, C₂H₅OH and FeCl₃ addition can be reproduced well by the Na₂CO₃, C₂H₅OH and Fe(CO)₅ sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achievedmainly by promoting the production of OH radicals at lower temperature.

关键词: Selective non-catalytic reduction, Denitrification, Ammonia, Kinetic modeling, O₂/CO₂, SO₂, Additives

Abstract: An experimental study of thermal de-NO_x using NH₃ as reductant in O₂/CO₂ atmosphere with the effect of SO₂ and different additiveswas performed in a drop tube furnace. Results show that the optimum temperature window is 841-1184℃, and the optimumreaction temperature is about 900℃ with a de-NO_x efficiency of 95.4%. A certain amount of SO₂ has an inhibiting effect on NO reduction. The effect of additives, including Na₂CO₃, C₂H₅OH and FeCl₃, on NO reduction by NH₃ is also explored. The addition of Na₂CO₃ and FeCl₃ is useful towiden the temperature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800℃. Qualitatively, the modeling results using a detailed kinetic modeling mechanism represent well most of the process features. The effect of Na₂CO₃, C₂H₅OH and FeCl₃ addition can be reproduced well by the Na₂CO₃, C₂H₅OH and Fe(CO)₅ sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achievedmainly by promoting the production of OH radicals at lower temperature.

Key words: Selective non-catalytic reduction, Denitrification, Ammonia, Kinetic modeling, O₂/CO₂, SO₂, Additives

Hui Li, Kuihua Han, Hongtao Liu, Chunmei Lu. Experimental and Modeling Study on de-NO_x Characteristics of Selective Non-catalytic Reduction in O₂/CO₂ Atmosphere[J]. Chinese Journal of Chemical Engineering, 2014, 22(8): 943-949.

Hui Li, Kuihua Han, Hongtao Liu, Chunmei Lu. Experimental and Modeling Study on de-NO_x Characteristics of Selective Non-catalytic Reduction in O₂/CO₂ Atmosphere[J]. Chin.J.Chem.Eng., 2014, 22(8): 943-949.

参考文献

[1] C.M. Nam, B.M. Gibbs, Application of the thermal deNO_x process to dieselengine deNO_x: an experimental and kinetic modeling study, Fuel 81 (2002)1359-1367.

[2] K.H. Han, C.M. Lu, Y.Z.Wang, N.S. Niu, Z.C. Liu,W.D. Hao, Experimental study on de-NO_x characteristics of selective non-catalytic reduction, Proc. Chin. Soc. Electron. Eng.28 (14) (2008) 80-85 (in Chinese).

[3] R. Rota, D. Antos, E.F. Zanoelo, M.Morbidelli, Experimental and modeling analysis ofthe NO_xOUT process, Chem. Eng. Sci. 57 (2002) 27-38.

[4] M.T. Javed, N. Irfan, B.M. Gibbs, Control of combustion-generated nitrogen oxides byselective non-catalytic reduction, J. Environ. Manag. 83 (2007) 251-289.

[5] D.L. Siebers, J.A. Caton, Removal of nitric oxide from exhaust gas with cyanuric acid,Combust. Flame 79 (1990) 31-46.

[6] P. Glarborg, P.G. Kristensen, S.H. Jensen, K.D. Johansen, A flow reactor study of HNCOoxidation chemistry, Combust. Flame 98 (1994) 241-258.

[7] G.W. Lee, B.H. Shon, J.G. Yoo, J.H. Jung, K.J. Oh, The influence of mixing between NH3 and NO for a de-NO_x reaction in the SNCR process, J. Ind. Eng. Chem. 14 (2008)457-467.

[8] W.H.J. Graus, E. Worrel, Effect of SO₂ and NOx control on energy-efficiency powergeneration, Energ Policy 35 (7) (2007) 3898-3908.

[9] W.J. Yang, Z.J. Zhou, J.H. Zhou, H.K. Lv, J.Z. Liu, K.F. Cen, Application of hybrid coalreburning/SNCR processes for NO_x reduction in a coal-fired boiler, Environ. Eng.Sci. 26 (2) (2009) 311-317.

[10] H.Y. Kim, S.W. Baek, C.Y. Lee, Effects of hybrid reburning system with SNCR and airstaging on NO_x reduction and thermal characteristics in oxygen enhanced combustion,Combust. Sci. Technol. 181 (10) (2009) 1289-1309.

[11] W.J. Yang, Z.C. Chen, Z.J. Zhou, Z.H. Wang, J.H. Zhou, Z.Y. Huang, K.F. Cen, Costefficientnitrogen oxides control by a hybrid selective noncatalytic reduction and selectivecatalytic reduction system on a utility boiler, Environ. Eng. Sci. 28 (5) (2011)341-348.

[12] K. Myöhänen, T. Hyppänen, T. Pikkarainen, T. Eriksson, A. Hotta, Near zero CO₂ emissionsin coal firing with oxy-fuel circulating fluidized bed boiler, Chem. Eng. Technol.32 (3) (2009) 355-363.

[13] Q.Z. Li, C.S. Zhao, W.F. Wu, X.P. Chen, W. Dong, Experimental investigation on NOemission characteristic during pulverized coal combustion in O₂/CO₂ environment,Proc. Chin. Soc. Electron. Eng. 29 (23) (2009) 33-39 (in Chinese).

[14] L.B. Duan, C.S. Zhao, J.Y. Lu,W. Zhou, Y.J. Li, X.P. Chen, SO₂/NO emission characteristicsduring O₂/CO₂ coal combustion process, J. Chem. Ind. Eng. Soc. China 60 (5)(2009) 1270-1274 (in Chinese).

[15] H. Liu, R. Zailani, B. Gibbs, Comparisons of pulverized coal combustion in air and inmixtures of O₂/CO₂, Fuel 84 (2005) 833-840.

[16] R. Zhao, H. Liu, H. Hu, X.J. Zhong, Z.J. Wang, Z.Y. Xu, J.R. Qiu, Experimental andmodeling study of NO emission under high CO₂ concentration, Sci. Chin. Technol.Sci. 53 (12) (2010) 3275-3283.

[17] Z.M. Lu, J.D. Lu, Influence of O₂ concentration on NO reduction and N₂O formation inthermal deNO_x process, Combust. Flame 156 (2009) 1303-1315.

[18] B.C. Moo, F.C. Chin, Low temperature SNCR process for NO_x control, Sci. Total Environ.198 (1997) 73-78.

[19] J.A. Miller, P. Glarborg, Modeling the formation of N₂O and NO₂ in the thermal de-NO_x process, in: M. Bodenstein, J. Wolfrum, H.R. Volppp, R. Rannacher, J. Warnatz(Eds.), Gas Phase Chemical Reaction Systems: Experiments and Models 100 YearsAfter, Springer Series in Chemical Physics, 1996, pp. 318-333.

[20] M.J. Pill, T. Turanyi, K.J. Hughes, “Irreversible mechanism mole Kelvin units”, TheUniversity of Leeds, http://garfield.chen.elte.hu/Combustion/mechanisms 2004.

[21] R. Rota, E.F. Zanoelo, Influence of oxygenated additives on the NO_xOUT process efficiency,Fuel 82 (2003) 765-770.

[22] V.M. Zamansky, V.V. Lissianski, P.M. Maly, L. Ho, D. Rusli,W.C. Gardiner, Reaction ofsodium species in the promoted SNCR process, Combust. Flame 117 (1999) 821-831.

[23] M.D. Rumminger, D. Reinelt, V. Babushok, G.T. Linteris, Numerical study of the inhibitionof premixed and diffusion flames by iron pentacarbonyl, Combust. Flame 116(1999) 207-219.

[24] A.E. Lutz, R.J. Kee, J.A. Miller, SENKIN: a FORTRAN program for predicting homogeneousgas phase chemical kinetics with sensitivity analysis, Sandia National LaboratoriesReport, SAND87-8248, 1988.

[25] D.M. Hamby, A review of techniques for parameter sensitivity analysis of environmentalmodels, Environ. Monit. Assess. 32 (2) (1994) 135-154.

[26] T. Turányi, Sensitivity analysis of complex kinetic systems. Tools and applications, J.Math. Chem. 5 (3) (1990) 203-248.

[27] S.H. Wu, Q.X. Cao, H. Liu, Q. An, X. Huang, Experimental and modeling study of theeffects of gas additives on the thermal deNO_x process, Chin. J. Chem. Eng. 18 (1)(2010) 143-148.

[28] L. Gasnot, D.Q. Dao, J.F. Pauwels, Experimental and kinetic study of the effect of additiveson the ammonia based SNCR process in low temperature conditions, EnergyFuel 26 (5) (2012) 2837-2849.

[29] S.L. Niu, K.H. Han, C.M. Lu, Experimental study on the effect of urea and additive injectionfor controlling nitrogen oxides emissions, Environ. Eng. Sci. 27 (1) (2010)47-53.

[30] J.A. Silver, The effect of sulfur on the thermal deNO_x process, Combust. Flame 53(1-3) (1983) 17-21.

[31] W.J. Yang, J.H. Zhou, J.J. Zhou, Z.C. Chen, J.Z. Liu, K.F. Cen, Action of oxygen and sodiumcarbonate in the urea-SNCR process, Combust. Flame 156 (2009) 1785-1790.

[32] K.H. Han, C.M. Lu, Kinetic model and simulation of promoted selective non-catalyticreduction by sodium carbonate, Chin. J. Chem. Eng. 15 (4) (2009) 512-519.

[33] S.L. Niu, K.H. Han, C.M. Lu, An experimental study on the effect of operating parametersand sodium additive on the NO_xOUT process, Process Saf. Environ. 89 (2011) 121-126.

[34] M.T. Javed, W. Nimmo, A. Mahmood, N. Irfan, Effect of oxygenated liquid additiveson the urea based SNCR process, J. Environ. Manag. 90 (2009) 3429-3435.

Experimental and Modeling Study on de-NO_x Characteristics of Selective Non-catalytic Reduction in O₂/CO₂ Atmosphere

Experimental and Modeling Study on de-NO_x Characteristics of Selective Non-catalytic Reduction in O₂/CO₂ Atmosphere

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