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

doi:10.1007/s11705-022-2224-5

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (4) : 460-469 https://doi.org/10.1007/s11705-022-2224-5

RESEARCH ARTICLE

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

Da Guo^1,², Guisheng Qi^1,²(

), Dong Chen^1,², Jiabao Niu^1,², Youzhi Liu^1,², Weizhou Jiao^1,²

¹. Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering, North University of China, Taiyuan 030051, China
². School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China

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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.

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

Corresponding Author(s): Guisheng Qi

Online First Date: 17 January 2023 Issue Date: 24 March 2023

Cite this article:

Da Guo,Guisheng Qi,Dong Chen, et al. Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate in the rotating packed bed[J]. Front. Chem. Sci. Eng., 2023, 17(4): 460-469.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2224-5
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I4/460

Fig.1 Schematic diagram of experimental setup (1. Steel cylinder for NO; 2. Steel cylinder for N₂; 3. Steel cylinder for O₂; 4. Valve unit; 5. Gas buffer tank; 6. Gas flow meter; 7. Homemade RPB; 8. Motor; 9. Solution storage tank; 10. Flue gas analyzer; 11. Liquid flow meter; 12. Pump; 13. Tail gas absorber).

Fig.2 Schematic diagram of RPB (7.1-rotor, 7.2-packing, 7.3-gas inlet, 7.4-shaft, 7.5-shaft seal, 7.6-liquid outlet, 7.7-cabinet, 7.8-gas outlet, 7.9-liquid distributor, 7.10-liquid inlet).

Fig.3 The influence of gas flow on η_NO (conditions: C_A (NO concentration) = 500 ppm, C_B ((NH₄)₂S₂O₈ concentration) = 0.1 mol·L^–1, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, pH = 4.50, Q_L (liquid flow) = 60 L·h^–1, β (high gravity factor) = 68.21, T = 293 K).

Fig.4 The effect of liquid–gas ratio on η_NO (conditions: C_A = 500 ppm, C_B = 0.1 mol·L^–1, pH = 4.50, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, Q_G = 1 m³·h^–1, β = 68.21, T = 293 K).

Fig.5 The influence of β on η_NO (conditions: C_A = 500 ppm, C_B = 0.1 mol·L^–1, pH = 4.50, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, Q_G = 1 m³·h^–1, L = 0.033, T = 293 K).

Fig.6 Effect of NO inlet concentration on η_NO (conditions: C_B = 0.1 mol·L^–1, pH = 4.50, Q_G = 1 m³·h^–1, L = 0.033, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, β = 77.61, T = 293 K).

Fig.7 Effect of (NH₄)₂S₂O₈ concentration on η_NO (conditions: C_A = 500 ppm, pH = 4.50, Q_G = 1 m³·h^–1, β = 77.61, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, L = 0.033, T = 293 K).

Fig.8 Linear fit between experimental value and calculated value.

Fig.9 The influence of O₂ on η_NO (conditions: C_A = 500 ppm, C_B = 0.1 mol·L^–1, pH = 4.50, Q_G = 1 m³·h^–1, L = 0.033, C (Fe²⁺-EDTA) = 0.01 mol·L^–1, β = 77.61, T = 293 K).

Fig.10 Changes in the concentration of iron in the solution: (a) Concentration of Fe²⁺, (b) Concentration of Fe³⁺.

Tab.1 Existence form of each substance after absorption^a)

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