Novel Process of Removal of Sulfur Dioxide by Aqueous Ammonia

Feb 15, 2016 - ABSTRACT: A novel wet flue gas desulfurization process by aqueous ammonia−fulvic acid solution was proposed, in which fulvic acid (FA...
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Novel Process of Removal of Sulfur Dioxide by Aqueous Ammonia-Fulvic Acid Solution with Ammonia Escape Inhibition Jitao Yang, Hanyang Gao, Guoxin Hu, Shiyuan Wang, and Ying Zhang Energy Fuels, Just Accepted Manuscript • DOI: 10.1021/acs.energyfuels.5b02555 • Publication Date (Web): 15 Feb 2016 Downloaded from http://pubs.acs.org on February 24, 2016

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Novel Process of Removal of Sulfur Dioxide by Aqueous Ammonia-Fulvic Acid Solution with Ammonia Escape Inhibition Jitao Yang†,‡, Hanyang Gao†, Guoxin Hu*,†, Shiyuan Wang‡, Ying Zhang‡ † School of Mechanical and Power Engineering, Shanghai Jiao Tong University, Shanghai 200240, China ‡ School of Energy and Environment Engineering, Zhongyuan University of Technology, Zhengzhou 450007, China

Abstract: A novel wet flue gas desulfurization process by aqueous ammonia-fulvic acid solution was proposed, in which fulvic acid (FA) could inhibit ammonia escape because carboxylic and phenolic groups in FA would interact with aqueous ammonia to form relatively stable ammonium fulvate. Experiments were conducted to research the effect of operating parameters such as initial pH value on the duration time of high efficiency (DTHE, time of above 95%) and absorption efficiency of SO2 in bubbling reactor. Results indicate that SO2 absorption efficiency and DTHE increase with increasing initial pH value, and SO2 absorption capacity of aqueous ammonia can be improved by synergic action of FA. FA concentration has slight effect on SO2 absorption efficiency (above 98.3%, pH0=8.5), but obvious effect on DTHE. FA can successfully inhibit ammonia escape from absorption liquid during desulfurization. When the pH of aqueous ammonia-FA absorption liquid is above 4.1, absorption *

Corresponding author phone/fax: +86-21-34206569; E-mail: [email protected].

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efficiency can be kept above 99.0% (for pH0=10.0). Increasing of inlet SO2 concentration brings the reduction of absorption efficiency and DTHE. High CO2 concentration is detrimental to DTHE. O2 and ammonium sulfate concentration hardly affect SO2 absorption efficiency and DTHE. Among nine operational parameters, gas flow rate has the biggest influence on overall gas-side volumetric mass transfer coefficient. The ammoniation of FA and mechanism of SO2 absorption in aqueous ammonia-fulvic acid solution also were demonstrated by FT-IR.

Keywords: flue gas desulfurization; SO2 absorption; aqueous ammonia; fulvic acid; ammoniation; pH 1. Introduction Sulfur dioxide emitted from coal-fired industrial and utility boilers is a major atmospheric pollutant that brings about detrimental influences on the environment and human health1. To alleviate SO2 emissions, air pollution engineers and researchers have attempted to develop various flue gas desulfurization (FGD) technologies, which mainly include ammonia2-4, catalytic oxidation5-6, seawater7, wet limestone or lime scrubbing8-9, organic amine10-11, semidry or dry adsorption12-13, metal ion solutions14 and dual-alkali method15. Among WFGD processes, ammonia-based WFGD has attracted increasing attentions in China in virtue of many excellent characteristics such as higher SO2 absorption efficiency, lower investment and valuable byproducts (ammonium sulfate fertilizer)16. However, in ammonia-based WFGD, ammonia escape and subsequent aerosol phenomena are fairly serious, which may result in abnormal operations of desulfurization devices and unacceptable high particle concentrations in exhaust gas17-18. Undoubtedly, ammonia escape can reduce the desulfurization capacity of absorbent. Hence, it is necessary to solve the problem of ammonia escape for a wide-scale industrial application of ammonia-based WFGD. Ammonia is a readily volatile compound characterized by a high saturated vapor pressure, a small density and a low boiling point19. Ammonium ion and hydroxide ion and un-ionized ammonia coexist in aqueous ammonia solution, and the corresponding equilibrium can be written as: NH + H O ⇌ NH ∙ H O ⇌ NH + OH 1 ACS Paragon Plus Environment

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Scheme 1

Scheme 2

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Inhibiting ammonia escape mechanism using FA.

Simplified scheme of FGD process by aqueous ammonia-fulvic acid solution proposed. (1)

prescrubber; (2) absorption tower; (3) liquid storage tank; (4, 5 and 7) pump; (6) oxidation tank; (8) spray dryer; (9) ammoniation tank. Because aqueous ammonia is weak alkaline, it could be used as absorption initiator of ammonia-based WFGD and compensate the decreasing pH of absorption liquid16. Ammonia escape is ACS Paragon Plus Environment

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dependent on the nature of NH3-SO2-H2O system, desulfurization operating conditions and desulfurization equipment. The usual approach of solving ammonia escape is to install the demister at the exit of the absorber or optimize the design of desulphurization tower and the operating conditions of desulfurization. For instance, Wang et al. carried out numerical simulation discussion of gas-liquid two-phase flow field for sintering flue gas in a wet ammonia-based FGD absorber by using ANSYS CFX, which supplied a reference for the design optimization of absorption tower17. Furthermore, ammonia escape phenomena could also be inhibited by modifying the nature of NH3-SO2-H2O system. Some investigations on adding chemical additives into aqueous ammonia solution such as ethanol20, sterically hindered amine21 and divalent metal ions22-24, have been reported. However, there are some questions for those additives, such as degradation, circulation loss, operation and raw material cost, etc. Fulvic acid (FA) that dissolves in water at any pH is one fraction of humic substances, which can be produced by the chemical and biological alteration of animal and plant tissue. FA has been known to be heterogeneous, consisting of numerous oxygen-containing functional groups, such as methoxyls, carboxyls, hydroxyls, carbonyls, and so on25-28. As two dominant functional groups that contribute to surface charge and reactivity of FA, carboxylic and phenolic groups can be protonated or deprotonated, which making FA behave as a polyelectrolyte29. The two weakly acidic groups (-COOH and -OH) are capable of interacting with aqueous ammonia to form soluble ammonium fulvate by ammoniation. Compared with aqueous ammonia, the formed ammonium fulvates are relatively stable, which could inhibit ammonia escape to some extent. Inhibiting ammonia escape mechanism using FA is presented in Scheme 128, 30. From the view of equilibrium 1, the amount of ammonia escaped depends on the concentration of free ammonia in the liquid phase. The binding of carboxylic and phenolic groups with ammonium ions could shift equilibrium 1 to the right and promote the dissolution and ionization of ammonia, consequently reducing the content of free ammonia in the liquid phase. Besides, free ammonia molecules could also be captured on FA by means of physical adsorption, which is attributed to high specific surface area of FA. But the physical adsorption of free ammonia is subordinate to chemical absorption of it. Ammonium fulvate is soluble and highly nutritive to plants like FA, namely, ACS Paragon Plus Environment

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fertilizer of outstanding quality for agriculture. However, fulvate can be protonated to FA under a strong acid condition. Because the acidity of SO2 (pKa1=1.8, sulfurous acid31) is higher than that of FA (pKa1=3.8, carboxyl groups32; pKa2=8.6, phenolic groups33-34), ammonium fulvate can indirectly interact with SO2, and the carboxylate and phenolate in FA can be protonated to carboxylic and phenolic groups. Therefore, in the present study, we propose a novel process of sulfur dioxide removal by aqueous ammonia-fulvic acid solution, please see Scheme 2. As shown in Scheme 2, this novel process has the following stages: (1) Ammoniation. Aqueous ammonia is added into FA solution in an ammoniation tank and stirred for some time. And then, the FA solution ammoniated is delivered to SO2 absorption liquid storage tank by pump. (2) Absorption of SO2. The flue gas continuously enters the spray tower at the bottom and upstream interacts with the aqueous slurry of FA ammoniated, and then continuously flows out at the top of tower. Because the flue gas in spray tower is the continuous phase, the pressure drop of tower is significantly lower than that of bubbling reactor. The FA solution ammoniated in liquid storage tank is pumped to the spray system of tower. In this counter current spray scrubber with small systemic resistance, the ammoniated FA solution can be distributed at different levels through a large number of nozzles that are fixed on horizontal spray headers35. SO2 gas dissolves in the aqueous slurry of FA ammoniated and initiates reactions with ammonium fulvate. Before departing from the absorber, the purified flue gas goes through the mist eliminator for the removal of slurry droplets entrained. Make-up water is supplied by the wash water from mist eliminator. The aqueous ammonia-fulvic acid solution loaded SO2 is collected at the bottom of absorber to complete absorption reactions. Part of absorption solution is circulated to spray zone by a circulating pump for reabsorbing SO2, until SO2 absorption efficiency has an obvious drop. A fresh aqueous ammonia-fulvic acid solution need be made up to absorption tower, when the FA ammoniated solution loses high SO2 absorption efficiency. (3) Oxidation. When the aqueous ammonia-fulvic acid solution has lost absorption efficiency, it is removed from absorption tower and transferred to oxidation tank in which ammonium sulfite will oxidized into ammonium sulfate. (4) Fertilizer. With a pump, the mixed solution of ammonium sulfate, FA and a few ammonium fulvate is delivered to spray dryer. After drying in spray dryer, the mixed solution is ACS Paragon Plus Environment

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processed into compound fertilizer, meanwhile water is recovered to ammoniation tank for the preparation of aqueous ammonia-fulvic acid solution. This novel process keeps ammonia from escaping through volatilization, but brings no secondary pollution by desulfurization additives or byproducts. Significantly, the byproducts of this process could be further processed into compound fertilizer containing ammonium sulfate, FA and ammonium fulvate. In this present work, we aim to investigate the impact of various operating parameters such as the initial pH value of aqueous ammonia-fulvic acid solution, FA concentration, O2 concentration, gas flow rate, absorption temperature, variation of pH value during desulfurization, inlet SO2 concentration, inlet CO2 concentration, fly ash and (NH4)2SO4 on SO2 absorption efficiency and desulfurization time in a lab-scale bubbling reactor, and achieve the optimal operating parameters for an efficient SO2-removal. Furthermore, we will verify the ammoniation of FA and the mechanism of SO2 absorption in aqueous ammonia-fulvic acid solution. This research is an essential preliminary to the application of aqueous ammonia-fulvic acid solution FGD process. 2. SO2 absorption mechanism According to the mechanism proposed by Hikita et al.36, we suppose a mechanism for the chemical absorption of sulfur dioxide by aqueous ammonia-fulvic acid solution, which are described in the following reactions. SO g ⇄ SO aq 2 SO aq + H O ⇌ H SO aq ⇌ HSO aq + H aq 3 

FA C6P > C6P^ > C\] > CG ). Note that QN has the biggest effect on the overall gas-side volumetric mass transfer coefficient, and next comes pH9. CG has the smallest effect on the overall gas-side volumetric mass transfer coefficient. The above results demonstrate that gas flow rate (correlation coefficient r = 0.994, p < 0.01) plays a critical role in the overall gas-side volumetric mass transfer coefficient. Meanwhile, three significantly negative correlations can be seen between T and K N aLG , CG and K N aLG , and C* and K N aLG , which are followed by six positive correlations. This indicates that the three operational parameters (temperature, inlet SO2 concentration, CO2 concentration) have a negative effect on the overall gas-side volumetric mass transfer coefficient. Therefore, the three operational parameters should be controlled to the low level for the improvement of overall gas-side volumetric mass transfer coefficient. Those unstandardized coefficients in Table 1 reflect the degree of nine predictor variables affecting 10_ K N aLG . For example, when the gas flow rate increases by 1 m h * , the overall gas-side volumetric mass transfer coefficient would increase by 41.892 × 10 _ mol m  s * Pa * ; pH9 increases by 1, and the overall gas-side volumetric mass transfer coefficient would increase by 0.031 × 10 _ mol m  s * Pa * . However, the overall gas-side volumetric mass transfer coefficient would decrease by 0.001 × 10 _ mol m  s * Pa * when the absorption temperature increases by 1 K. Fig. 13 shows the comparison between the experimental K N aLG and predicted K N aLG values by the regression equation 28. From Fig. 13, it can be observed

that

the

experimental

K N aLG

values

lie

within

the

range

from 4.3 × 10 _ to 7.2 × 10 _ mol m  s * Pa * , and the maximum relative deviation between the experimental K N aLG and predicted K N aLG values is 1%. The regression equation 28 shows a good accuracy with the experimental values, so it may provide a reference for the design of SO2 bubbling absorption in aqueous ammonia-FA blend solution. 4.13 FT-IR analysis ACS Paragon Plus Environment

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600

1713

I

1770

II Transmittance (%)

hydrogen-bonded O-H stretching and N-H stretching

3500

3000

2500

2000

1500

1000

531

1600 1517 1460 1426 1330 1219 1118 1043 915

2940

1705 υC=O(COOH)

654

2844

III

3405

500

-1

Wavenumber (cm )

IR spectra of ammonia-FA+SO2 (I), FA after ammoniation (II) and FA before ammoniation (III). 1770 1713, υ (COOH) C=O I 1404 + NH4 1606

II

1404 + NH4 1705 υC=O(COOH)

1800

III

1600

(a)

Transmittance (%)

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1700 1600 1500 -1 Wavenumber (cm )

1400

(b) The partial enlargement of Fig. 14(a).

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Fig. 14

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IR spectra of ammonia-FA+SO2 (I), FA after ammoniation (II) and FA before ammoniation

(III). ammonia-FA+SO2: ammonia-FA desulfurization products (experiment condition, 100 mL 4g FA + aqueous ammonia solution, pH0=8.5; gas flow of 0.14 m3 h-1; inlet SO2 concentration of 2000 ppm; CO2 of 15%; O2 of 5%; at 25 °C. When SO2 absorption efficiency dropped to 75%, the SO2 absorption experiment was terminated). Fig. 14 shows the result of FT-IR spectra of FA+SO2, FA after and before ammoniation. As shown in Fig. 14, the FT-IR spectra of the three samples look fairly similar and appear the uniform pattern of absorption bands. Nevertheless, there are still obvious differences among the three spectra. Based on previous researches38, 52-64, the spectra of FA before ammoniation can be interpreted as below. The broad and intense absorption band at 3405 cm-1 is assigned to the hydrogen-bonded O-H stretching (phenols, carboxyls and alcohols) and N-H stretching (amides and amines)38, 52-54. The 2940 and 2844 cm-1 bands are attributed to the symmetric and asymmetric stretching vibrations of aliphatic C-H bond (in CH2 and CH3)53-54. For the shoulder band at 1705 cm-1, it represents the contribution from the υb COOH stretching38, 55, 65. The intense absorption peak at 1600 cm-1 corresponds to the C=C vibration of aromatic structures and the asymmetric C=O stretching of COO group38, 54-55. The 1460 cm-1 band can be ascribed to the C-H stretching of CH2 and CH3 groups of aliphatic chains56-57. The 1426 cm-1 absorption belongs to the symmetrical C=O stretching of COO group and aliphatic C-H bendings58-59, and the 1330 cm-1 is related to the syringyl ring breathing with C-O stretching57, 61. The intense band appears at 1219 cm-1, which can represent contributions from the C-O stretching and O-H deformation of -COOH52, 60. The band at 1118 cm-1 is caused by the aromatic C-H in plane deformation (syringyl)61. The 1043 cm-1 is due to the alcoholic and polysaccharide C-O stretch and O-H deformation62, including sulfonic acids63. Additionally, the 654 cm-1 in the fingerprint region corresponds to the S-O stretching of sulphonic group64. Interestingly, the FT-IR spectra of FA after ammoniation changes greatly. As observed in Fig. 14, the shoulder at 1705 cm-1 completely disappears, while another new weak shoulder that can represent the contribution from a symmetric bending vibration of NH group appears at 1404 cm-166-67, and the band at 3405 cm-1 becomes narrow after ACS Paragon Plus Environment

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ammoniation. It indicates that the carboxylic (-COOH) and phenolic (-OH) groups in FA have been transformed into deprotonated carboxylate (-COO－) and phenolate (-O－) groups38. Namely, FA has 

been transformed into ammonium fulvate (FA 99.0%), the pH of aqueous ammonia-FA absorption liquid is suggested to be above 4.1. (6) The increase of inlet SO2 concentration can cause the slight reduction of SO2 absorption efficiency and DTHE. (7) The variation of CO2 concentration from 0 to 15 % hardly affects the SO2 absorption efficiency in the beginning of absorption, but high CO2 concentration is detrimental to the SO2 removal from flue gas. (8) High fly ash concentration can improve the SO2 removal capability of aqueous ammonia-FA solution. (9) Ammonium sulfate concentration hardly impacts the SO2 absorption efficiency and DTHE. (10) Among nine operational parameters, gas flow rate has the biggest effect on the overall gas-side volumetric mass transfer coefficient. Besides, the ammoniation of FA and the mechanism of SO2 absorption in aqueous ammonia-fulvic acid solution have been verified by FT-IR. This novel WFGD process can not only prevent ammonia ACS Paragon Plus Environment

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from escaping by way of volatilization, but also produce the byproducts containing ammonium sulfate, FA and ammonium fulvate, which could be further processed into compound fertilizer for agriculture. So, the removal of SO2 by ammonia-fulvic acid solution could be a promising WFGD process. Acknowledgements We gratefully acknowledge financial support by the National Agriculture Science Technology Achievement Transformation Fund of China (2013GB23600665). We also thank Instrumental Analysis Center of SJTU for FT-IR. References (1) Huang, K.; Lu, J.-F.; Wu, Y.-T.; Hu, X.-B.; Zhang, Z.-B., Absorption of SO2 in aqueous solutions of mixed hydroxylammonium dicarboxylate ionic liquids. Chem. Eng. J. 2013, 215–216, 36. (2) Bai, H.; Biswas, P.; Keener, T. C., SO2 removal by NH3 gas injection: effects of temperature and moisture content. Ind. Eng. Chem. Res. 1994, 33, 1231. (3) He, B.; Zheng, X.; Wen, Y.; Tong, H.; Chen, M.; Chen, C., Temperature impact on SO2 removal efficiency by ammonia gas scrubbing. Energy Convers. Manage. 2003, 44, 2175. (4) Gao, X.; Du, Z.; Ding, H. L.; Wu, Z. L.; Lu, H.; Luo, Z. Y.; Cen, K. F., Kinetics of NOx absorption into (NH4)2SO3 solution in an ammonia-based wet flue gas desulfurization process. Energy Fuels 2010, 24, 5876. (5) Vernikovskaya, N. V.; Zagoruiko, A. N.; Noskov, A. S., SO2 oxidation method. Mathematical modeling taking into account dynamic properties of the catalyst. Chem. Eng. Sci. 1999, 54, 4475. (6) Jiang, J.-H.; Li, Y.-H.; Cai, W.-M., Experimental and mechanism research of SO2 removal by cast iron scraps in a magnetically fixed bed. J. Hazard. Mater. 2008, 153, 508. (7) Vidal B, F.; Ollero, P.; Gutierrez Ortiz, F.; Villanueva, A., Catalytic seawater flue gas desulfurization process: an experimental pilot plant study. Environ. Sci. Technol. 2007, 41, 7114.

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