A composite absorption liquid for simultaneous desulfurization and denitrification in flue gas

doi:10.1016/j.cjche.2019.04.013

摘要/Abstract

摘要： A composite-liquid absorbent (CLA), NaClO/KMnO₄, for simultaneous desulfurization and denitrification (SDD) was studied in a homemade bubbling reactor. The experimental results showed that the CLA configured by sodium hypochlorite (NaClO) and potassium permanganate (KMnO₄) had a very good synergistic effect on SDD. The effects of NaClO concentration (C_Na), KMnO₄ concentration (C_K), gas space velocity (V_g), initial pH value, and temperature of the absorption liquid (T_s) on efficiencies of the SDD were investigated. Under the optimal reaction conditions, the best removal efficiencies were 100% for sulfur dioxide (SO₂) and above 94% for nitric oxide (NO). The ion chromatography and titration were used to analyze the changes of both the ion species and concentrations in the liquid before and after the reaction. According to the experiment results and related literature, the reaction mechanism of the SDD based on the CLA was proposed.

关键词: Flue gas, Absorption, Chemical reaction, Reaction mechanism, NaClO/KMnO₄

Abstract: A composite-liquid absorbent (CLA), NaClO/KMnO₄, for simultaneous desulfurization and denitrification (SDD) was studied in a homemade bubbling reactor. The experimental results showed that the CLA configured by sodium hypochlorite (NaClO) and potassium permanganate (KMnO₄) had a very good synergistic effect on SDD. The effects of NaClO concentration (C_Na), KMnO₄ concentration (C_K), gas space velocity (V_g), initial pH value, and temperature of the absorption liquid (T_s) on efficiencies of the SDD were investigated. Under the optimal reaction conditions, the best removal efficiencies were 100% for sulfur dioxide (SO₂) and above 94% for nitric oxide (NO). The ion chromatography and titration were used to analyze the changes of both the ion species and concentrations in the liquid before and after the reaction. According to the experiment results and related literature, the reaction mechanism of the SDD based on the CLA was proposed.

Key words: Flue gas, Absorption, Chemical reaction, Reaction mechanism, NaClO/KMnO₄

Chunlai Liu, Jing Li, Changlin Yang, Zhenheng Diao, Chengxue Wang. A composite absorption liquid for simultaneous desulfurization and denitrification in flue gas[J]. 中国化学工程学报, 2019, 27(10): 2566-2573.

Chunlai Liu, Jing Li, Changlin Yang, Zhenheng Diao, Chengxue Wang. A composite absorption liquid for simultaneous desulfurization and denitrification in flue gas[J]. Chinese Journal of Chemical Engineering, 2019, 27(10): 2566-2573.

参考文献

[1] X. Wu, K. Wu, Y. Zhang, et al., Comparative life cycle assessment and economic analysis of typical flue-gas cleaning processes of coal-fired power plants in China, J. Clean. Prod. 142(2017) 3236-3242.
[2] Z. Song, B. Wang, J. Yu, et al., Density functional study on the heterogeneous oxidation of NO over α-Fe₂O₃ catalyst by H₂O₂:Effect of oxygen vacancy, Appl. Surf. Sci. 413(2017) 292-301.
[3] Y. Zhao, T. Guo, Z. Chen, Experimental study on simultaneous desulfurization and denitrification from flue gas with composite absorbent, Environ. Prog. Sustain. Energy 30(2) (2011) 216-220.
[4] Y. Zhao, R.L. Hao, Q. Guo, et al., Simultaneous removal of SO₂ and NO by a vaporized enhanced-Fenton reagent, Fuel Process. Technol. 137(2015) 8-15.
[5] X. Huang, J. Ding, Q. Zhong, Catalytic decomposition of H₂O₂ over Fe-based catalysts for simultaneous removal of NO_X and SO₂, Appl. Surf. Sci. 326(2015) 66-72.
[6] Y. Zhao, Y. Han, T. Ma, T. Guo, Simultaneous desulfurization and denitrification from flue gas by Ferrate (VI), Environ. Sci. Technol. 45(9) (2011) 4060-4065.
[7] G.X. Hu, Z.G. Sun, H.Y. Gao, Novel process of simultaneous removal of SO₂ and NO₂ by sodium humate solution, Environ. Sci. Technol. 44(17) (2010) 6712-6717.
[8] A. Pourmohammadbagher, E. Jamshidi, H. Ale-Ebrahim, S. Dabir, Study on simultaneous removal of NO_x and SO₂ with NaClO₂ in a novel swirl wet system, Ind. Eng. Chem. Res. 50(13) (2011) 8278-8284.
[9] P. Fang, C. Cen, Z. Tang, et al., Simultaneous removal of SO₂ and NO_X by wet scrubbing using urea solution, Chem. Eng. J. 168(2011) 52-59.
[10] Y. Zhao, F. Liu, T. Guo, et al., Experiments and reaction characteristics of liquid phase simultaneous removal of SO₂ and NO, Sci. China, Ser. E:Technol. Sci. 52(6) (2009) 1768-1775.
[11] Y. Zhao, F. Liu, T. Guo, et al., Reaction kinetics of simultaneous removal of SO₂ and NO from flue gas by NaClO₂ solution, Int. J. Chem. React. Eng. 9(1) (2011) 1-15.
[12] J. Zhang, R. Zhang, X. Chen, et al., Simultaneous removal of NO and SO₂ from flue gas by ozone oxidation and NaOH absorption, Ind. Eng. Chem. Res. 53(15) (2014) 6450-6456.
[13] Y. Zhao, R. Hao, P. Zhang, et al., Integrative process for simultaneous removal of SO₂ and NO utilizing a vaporized H₂O₂/Na₂S₂O₈, Energy Fuel 28(10) (2014) 6502-6510.
[14] D. Zhang, H. Tao, C. Yao, et al., Effects of residence time on the efficiency of desulfurization and denitrification in the bubbling reactor, Chem. Eng. Sci. 174(2017) 203-221.
[15] B.M. Sun, S.E. Yin, Z.L. Wang, Study on the experiments of flue gas denitrification and desulfurization using nitric acid solution, ASME International Conference on Energy Sustainability Collocated with the Heat Transfer 2008, pp. 239-246.
[16] R. Hao, S. Yang, B. Yuan, et al., Simultaneous desulfurization and denitrification through an integrative process utilizing NaClO₂/Na₂S₂O₈, Fuel. Process. Technol. 159(2017) 145-152.
[17] J. Wang, W.Q. Zhong, Simultaneous desulfurization and denitrification of sintering flue gas via composite absorbent, Chin. J. Chem. Eng. 24(8) (2016) 1104-1111.
[18] Y. Zhao, R. Hao, B. Yuan, et al., Simultaneous removal of SO₂, NO and Hg (0) through an integrative process utilizing a cost-effective complex oxidant, J. Hazard. Mater. 301(2016) 74-83.
[19] Q. Du, H. Zhao, L. Ming, et al., Experimental investigation on the kinetics of NO complex absorption through FeIIEDTA solvent in a double-stirred reactor, Ind. Eng. Chem. Res. 50(8) (2011) 4425-4431.
[20] Y. Zhao, T. Guo, Z. Zang, Activity and characteristics of "Oxygen-enriched" highly reactive absorbent for simultaneous flue gas desulfurization and denitrification, Front. Environ. Sci. Eng. 9(2) (2014) 222-229.
[21] H.J. Yoon, H.W. Park, D.W. Park, Simultaneous oxidation and absorption of NO_x and SO₂ in an integrated O₃ oxidation/wet atomizing system, Energy Fuel 30(4) (2016) 3289-3297.
[22] M. Bai, Z. Zhang, M. Bai, Simultaneous desulfurization and denitrification of flue gas by·OH radicals produced from O²⁺ and water vapor in a duct, Environ. Sci. Technol. 46(18) (2012) 10161-10168.
[23] J. Ding, H. Cai, Q. Zhong, et al., Selective denitrification of flue gas by O₃ and ethanol mixtures in a duct:Investigation of processes and mechanisms, J. Hazard. Mater. 311(2016) 218-229.
[24] Z. Han, S. Yang, X. Pan, et al., New experimental results of NO removal from simulated flue gas by wet scrubbing using NaClO solution, Energy Fuel 31(3) (2017) 3047-3054.
[25] Y. Li, W. Zhong, J. Ju, et al., Experiment on simultaneous absorption of NO and SO₂ from sintering flue gas by oxidizing agents of KMnO₄/NaClO, Int. J. Chem. React. Eng. 12(1) (2014) 539-547.
[26] M.C. Pereira, L.C.A. Oliveira, E. Murad, Iron oxide catalysts:Fenton and Fenton-like reactions-A review, Clay Miner. 47(3) (2018) 285-302.
[27] L.Z. Zhai, Q. Zhong, X.R. Wang, Experimental research on flue gas desulfurization with ethylenediamine, Adv. Mater. Res. 356-360(2011) 1723-1727.
[28] Y. Zhou, C. Li, C. Fan, et al., Wet removal of sulfur dioxide and nitrogen oxides from simulated flue gas by Ca(ClO)2 solution, Environ. Prog. Sustain. Energy 34(6) (2015) 1586-1595.
[29] Z.L. Xin, J.L. Zhang, H.L. Xu, et al., Experimental study on removal of NO from flue gas in aqueous triethylenetetraminecobalt solution, Chemical Engineering (China) 39(6) (2011) 8-11.
[30] H. Ping, Technological comparison of sprinkling tower and bubbling tower type wet FGD process, Jiangxi Electric Power 30(5) (2004) 1-3.
[31] Z.S. Wei, H.J. Niu, Y.F. Ji, Simultaneous removal of SO₂ and NO_X by microwave with potassium permanganate over zeolite, Fuel Process. Technol. 90(2) (2009) 324-329.
[32] Z.M. Zhang, H.C. Sheng, X.X. Lin, et al., Experimental study on simultaneous desulfurization and denitrification by KMnO₄ oxidation combining NaOH liquid absorption, Environ. Eng. 35(8) (2017) 102-107.
[33] K.M. Monoj, R.C. Vaishnava, New experimental results of combined SO₂ and NO removal from simulated gas stream by NaClO as low-cost absorbent, Chem. Eng. J. 217(2013) 48-53.
[34] J. Meng, Research progress of the control of manganiferous waste water, Journal of Anhui Agri. Sci. 36(32) (2008) 14273-14274.
[35] B.J. Liu, L.Y. Zhang, M.Y. Tao, et al., Removing chloride in sample of COD with silver nitrate, The Administration and Technique of Environmental Monitoring 8(6) (1996) 38-39.
[36] H.Y. Wang, S.L. Xu, Present status of technology for production of potassium sulfate, Chemical Fertilizer Industry 32(1) (2005) 29-31.
[37] H.Y. Li, X.F. Wang, Effect of nitrate fertilizer on abscisic acid content and chloroplast ultrastructure of cucumber leaf, Plant Nutrition and Fertilizer Science 10(3) (2004) 324-326.
[38] L.J. Muzio, G.C. Quartucy, J.E. Cichanowiczy, Overview and status of post-combustion NO_x control:SNCK SCR and hybrid technologies, Int. J. Environ. Pollut. 17(1-2) (2002) 4-30.
[39] Z.Y. Yu, W. Yan, L.L. Zhang, et al., Deactivation mechanism and regeneration methods of SCR de-NO_x catalysts, Boiler Technology 49(6) (2018) 73-78.