Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate in the rotating packed bed

Abstract

Nitric oxide being a major gas pollutant has attracted much attention and various technologies have been developed to reduce NO emission to preserve the environment. Advanced persulfate oxidation technology is a workable and effective choice for wet flue gas denitrification due to its high efficiency and green advantages. However, NO absorption rate is limited and affected by mass transfer limitation of NO and aqueous persulfate in traditional reactors. In this study, a rotating packed bed (RPB) was employed as a gas–liquid absorption device to elevate the NO removal efficiency (η_NO) by aqueous persulfate ((NH₄)₂S₂O₈) activated by ferrous ethylenediaminetetraacetate (Fe²⁺-EDTA). The experimental results regarding the NO absorption were obtained by investigating the effect of various operating parameters on the removal efficiency of NO in RPB. Increasing the concentration of (NH₄)₂S₂O₈ and liquid–gas ratio could promoted the oxidation and absorption of NO while theη_NO decreased with the increase of the gas flow and NO concentration. In addition, improving the high gravity factor increased the η_NO and the total volumetric mass transfer coefficient (K_Gα) which raise the η_NO up to more than 75% under the investigated system. These observations proved that the RPB can enhance the gas–liquid mass transfer process in NO absorption. The correlation formula between K_Gα and the influencing factors was determined by regression calculation, which is used to guide the industrial scale-up application of the system in NO removal. The presence of O₂ also had a negative effect on the NO removal process and through electron spin resonance spectrometer detection and product analysis, it was revealed that Fe²⁺-EDTA activated (NH₄)₂S₂O₈ to produce •SO₄^–, •OH and •O₂^–, played a leading role in the oxidation of NO, to produce NO₃^– as the final product. The obtained results demonstrated a good applicable potential of RPB/PS/Fe²⁺-EDTA in the removal of NO from flue gases.

Graphical abstract

Keywords

rotating packed bed / Fe²⁺-EDTA / sulfate radical / hydroxyl radical / NO removal efficiency

References

[1] Meng Z, Wang C, Wang X, Chen Y, Wu W, Li H. Simultaneous removal of SO₂ and NO_x from flue gas using (NH₄)₂S₂O₃/steel slag slurry combined with ozone oxidation. Fuel, 2019, 255: 115760

[2] Chen X, Hu X, Gao Y. Removal of NO in simulated flue with aqueous solution of peroxymonosulfate activated by high temperature and Fe(II). Chemical Engineering Journal, 2019, 359: 419–427

[3] Adewuyi Y G, Khan M A. Nitric oxide removal from flue gas by combined persulfate and ferrous-EDTA solutions: effects of persulfate and EDTA concentrations, temperature, pH and SO₂. Chemical Engineering Journal, 2016, 304: 793–807

[4] Hao R, Wang X, Mao X, Tian B, Zhao Y, Yuan B, Tao Z, Shen Y. An integrated dual-reactor system for simultaneous removal of SO₂ and NO: factors assessment, reaction mechanism and application prospect. Fuel, 2018, 220: 240–247

[5] Hao R, Mao Y, Mao X, Wang Z, Gong Y, Zhang Z, Zhao Y. Cooperative removal of SO₂ and NO by using a method of UV-heat/H₂O₂ oxidation combined with NH₄OH-(NH₄)₂SO₃ dual-area absorption. Chemical Engineering Journal, 2019, 365: 282–290

[6] Adewuyi Y G, Sakyi N Y, Arif Khan M. Simultaneous removal of NO and SO₂ from flue gas by combined heat and Fe²⁺ activated aqueous persulfate solutions. Chemosphere, 2018, 193: 1216–1225

[7] Huang H, Hu H, Fan M, Chen J, Yuan S, Annanurov S. Mechanistic research on NO removal by K₂S₂O₈ with electrochemical catalysis. Chemical Engineering Journal, 2020, 382: 122873

[8] Liu Y, Zhang J, Pan J, Tang A. Investigation on removal of NO from SO₂-containing simulated flue gas by UV/Fenton-like reaction. Energy & Fuels, 2012, 26(9): 5430–5436

[9] Li G, Wang B, Xu W Q, Li Y, Han Y, Sun Q. Simultaneous removal of SO₂ and NO_x from flue gas by wet scrubbing using a urea solution. Environmental Technology, 2019, 40(20): 2620–2632

[10] Wang L, Zhao W, Wu Z. Simultaneous absorption of NO and SO₂ by Fe^II-EDTA combined with Na₂SO₃ solution. Chemical Engineering Journal, 2007, 132(1–3): 227–232

[11] Zhang Q, Wang S, Zhang G, Wang Z, Zhu P. Effects of slurry properties on simultaneous removal of SO₂ and NO by ammonia-Fe(II)EDTA absorption in sintering plants. Journal of Environmental Management, 2016, 183: 1072–1078

[12] Zhao Y, Guo T, Chen Z, Du Y. Simultaneous removal of SO₂ and NO using M/NaClO₂ complex absorbent. Chemical Engineering Journal, 2010, 160(1): 42–47

[13] Han Z, Yang S, Pan X, Zhao D, Yu J, Zhou Y, Xia P, Zheng D, Song Y, Yan Z. New experimental results of NO removal from simulated flue gas by wet scrubbing using NaClO solution. Energy & Fuels, 2017, 31(3): 3047–3054

[14] Han Z, Gao Y, Yang S, Dong J, Pan X, Lan T, Song L, Yan Z, Sun D, Ning K N O. Removal from simulated diesel engine exhaust gas by cyclic scrubbing using NaClO₂ solution in a rotating packed bed reactor. Journal of Chemistry, 2019, 2019: 1–9

[15] Chu H, Chien T W, Li S Y. Simultaneous absorption of SO₂ and NO from flue gas with KMnO₄/NaOH solutions. Science of the Total Environment, 2001, 275(1–3): 127–135

[16] Shahrestani M M, Rahimi A, Momeni M. Experimental study and mathematical modeling of NO removal using the UV/H₂O₂ advanced oxidation process. Chemical Engineering & Technology, 2017, 40(6): 1149–1157

[17] Liu Y, Wang Y. Simultaneous removal of NO and SO₂ using aqueous peroxymonosulfate with coactivation of Cu²⁺/Fe³⁺ and high temperature. AIChE Journal, 2017, 63(4): 1287–1302

[18] Wang Z, Wang Z, Ye Y, Chen N, Li H. Study on the removal of nitric oxide (NO) by dual oxidant (H₂O₂/S₂O₈^2–) system. Chemical Engineering Science, 2016, 145: 133–140

[19] Adewuyi Y G, Sakyi N Y. Removal of nitric oxide by aqueous sodium persulfate simultaneously activated by temperature and Fe²⁺ in a lab-scale bubble reactor. Industrial & Engineering Chemistry Research, 2013, 52(41): 14687–14697

[20] Adewuyi Y G, Sakyi N Y. Simultaneous absorption and oxidation of nitric oxide and sulfur dioxide by aqueous solutions of sodium persulfate activated by temperature. Industrial & Engineering Chemistry Research, 2013, 52(33): 11702–11711

[21] Liu Y, Liu Z, Wang Y, Yin Y, Pan J, Zhang J, Wang Q. Simultaneous absorption of SO₂ and NO from flue gas using ultrasound/Fe²⁺/heat coactivated persulfate system. Journal of Hazardous Materials, 2018, 342: 326–334

[22] Zhen G, Lu X, Wang B, Zhao Y, Chai X, Niu D, Zhao A, Li Y, Song Y, Cao X. Synergetic pretreatment of waste activated sludge by Fe(II)-activated persulfate oxidation under mild temperature for enhanced dewaterability. Bioresource Technology, 2012, 124: 29–36

[23] Adewuyi Y G, Khan M A, Sakyi N Y. Kinetics and modeling of the removal of nitric oxide by aqueous sodium persulfate simultaneously activated by temperature and Fe²⁺. Industrial & Engineering Chemistry Research, 2014, 53(2): 828–839

[24] Chen L, Ma J, Li X, Zhang J, Fang J, Guan Y, Xie P. Strong enhancement on fenton oxidation by addition of hydroxylamine to accelerate the ferric and ferrous iron cycles. Environmental Science & Technology, 2011, 45(9): 3925–3930

[25] Liang C, Bruell C J, Marley M C, Sperry K L. Persulfate oxidation for in situ remediation of TCE. II. Activated by chelated ferrous ion. Chemosphere, 2004, 55(9): 1225–1233

[26] Adewuyi Y G, Khan M A. Nitric oxide removal by combined persulfate and ferrous-EDTA reaction systems. Chemical Engineering Journal, 2015, 281: 575–587

[27] Khan N E, Adewuyi Y G. Absorption and oxidation of nitric oxide (NO) by aqueous solutions of sodium persulfate in a bubble column reactor. Industrial & Engineering Chemistry Research, 2010, 49(18): 8749–8760

[28] Gao X, Ma X, Kang X, Shi Y. Oxidative absorption of NO by sodium persulfate coupled with Fe²⁺, Fe₃O₄, and H₂O₂. Environmental Progress & Sustainable Energy, 2015, 34(1): 117–124

[29] Liu Y, Wang Y. Simultaneous removal of NO and SO₂ using aqueous peroxymonosulfate with coactivation of Cu²⁺/Fe³⁺ and high temperature. AIChE Journal, 2017, 63(4): 1287–1302

[30] Chen X, Hu X. Kinetics of the removal of NO using PMS-Fe(II) system activated by high temperature and Fe(II) ions in the multi-stage stirred bubble reactor. Chemical Engineering Journal, 2020, 379: 122144

[31] Luo Y, Chu G, Zou H, Zhao Z, Dudukovic M P, Chen J. Gas−liquid effective interfacial area in a rotating packed bed. Industrial & Engineering Chemistry Research, 2012, 51(50): 16320–16325

[32] Zhao H, Shao L, Chen J. High-gravity process intensification technology and application. Chemical Engineering Journal, 2010, 156(3): 588–593

[33] Zhang L, Wang J, Sun Q, Zeng X, Chen J. Removal of nitric oxide in rotating packed bed by ferrous chelate solution. Chemical Engineering Journal, 2012, 181–182: 624–629

[34] Guo J, Jiao W, Qi G, Yuan Z, Liu Y. Applications of high-gravity technologies in gas purifications: a review. Chinese Journal of Chemical Engineering, 2019, 27(6): 1361–1373

[35] Sandilya P, Rao D P, Sharma A, Biswas G. Gas-phase mass transfer in a centrifugal contactor. Industrial & Engineering Chemistry Research, 2001, 40(1): 384–392

[36] Adewuyi Y G, He X, Shaw H, Lolertpihop W. Simultaneous absorption and oxidation of NO and SO₂ by aqueous solutions of sodium chlorite. Chemical Engineering Communications, 1999, 174(1): 21–51

[37] Liu Y, Wang Y, Xu W, Yang W, Pan Z, Wang Q. Simultaneous absorption−oxidation of nitric oxide and sulfur dioxide using ammonium persulfate synergistically activated by UV-light and heat. Chemical Engineering Research & Design, 2018, 130: 321–333

[38] Li Y, Liu Y, Zhang L, Su Q, Jin G. Absorption of NO_x into nitric acid solution in rotating packed bed. Chinese Journal of Chemical Engineering, 2010, 18(2): 244–248

[39] Jiao W, Liu Y, Qi G. A new impinging stream-rotating packed bed reactor for improvement of micromixing iodide and iodate. Chemical Engineering Journal, 2010, 157(1): 168–173

[40] Romero A, Santos A, Vicente F, González C. Diuron abatement using activated persulphate: effect of pH, Fe(II) and oxidant dosage. Chemical Engineering Journal, 2010, 162(1): 257–265

[41] Wang Q, Shao Y, Gao N, Chu W, Deng J, Shen X, Lu X, Zhu Y, Wei X. Degradation of alachlor with zero-valent iron activating persulfate oxidation. Journal of the Taiwan Institute of Chemical Engineers, 2016, 63: 379–385

[42] Chen X, Hu X. Removal of NO_x and SO₂ from the coal-fired flue gas using a rotating packed bed pilot reactor with peroxymonosulfate activated by Fe(II) and heating. Energy & Fuels, 2019, 33(7): 6707–6716

[43] Adewuyi Y G, Khan M A. Simultaneous NO and SO₂ removal by aqueous persulfate activated by combined heat and Fe²⁺: experimental and kinetic mass transfer model studies. Environmental Science and Pollution Research International, 2020, 27(2): 1186–1201

[44] Liu N, Lu B, Zhang S, Jiang J, Cai L, Li W, He Y. Evaluation of nitric oxide removal from simulated flue gas by Fe(II)EDTA/Fe(II)citrate mixed absorbents. Energy & Fuels, 2012, 26(8): 4910–4916

[45] Gambardella F, Winkelman J G M, Heeres H J. Experimental and modelling studies on the simultaneous absorption of NO and in aqueous iron chelate solutions. Chemical Engineering Science, 2006, 61(21): 6880–6891

[46] Hao R, Yang S, Yuan B, Zhao Y. Simultaneous desulfurization and denitrification through an integrative process utilizing NaClO₂/Na₂S₂O₈. Fuel Processing Technology, 2017, 159: 145–152

[47] Furman O S, Teel A L, Watts R J. Mechanism of base activation of persulfate. Environmental Science & Technology, 2010, 44(16): 6423–6428

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