Abstract
Hg0, SO2, and NOx result in heavily global environmental pollution and serious health hazards. Up to now, how to efficiently remove mercury with SO2 and NOx from flue gas is still a tough task. In this study, series of high oxidizing Fenton systems were employed to purify the pollutants. The experimental results showed that Fe3+/H2O2 was more suitable to purify Hg0 than Fe2+/H2O2 and Cu2+/H2O2. The optimal condition includes Fe3+ concentration of 0.008 mol/L, Hg0 inlet concentration of 40 μg/m3, solution temperature of 50 °C, pH of 3, H2O2 concentration of 0.7 mol/L, and O2 percentage of 6%. When SO2 and NOx were taken into account under the optimal condition, Hg0 removal efficiency could be enhanced to 91.11% while the removal efficiency of both NOx and SO2 was slightly declined, which was consistent to the analysis of purifying mechanism. The removal efficiency of Hg0 was stimulated by accelerating the conversion of Fe2+ to Fe3+, which resulted from the existence of SO2 and NOx. The results of this study suggested that simultaneously purifying Hg0, SO2, and NOx from flue gas is feasible.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Bobu M, Yediler A, Siminiceanu I, Schulte-Hostede S (2008) Degradation studies of ciprofloxacin on a pillared iron catalyst. Appl Catal B Environ 83(1-2):15–23. https://doi.org/10.1016/j.apcatb.2008.01.029
Boiko VM (2003) Rates of hydroxyl radical generation and organic compound oxidation in mineral-catalyzed Fenton-like systems. Environ Sci Technol 37:1150–1158
Byun Y, Hamilton LP, Xin T, Dong NS (2014) Formation of chlorinated species through reaction of SO2 with NaClO2 powder and their role in the oxidation of NO and Hg0. Environ Sci Pollut Res 21(13):8052–8058. https://doi.org/10.1007/s11356-014-2669-2
Carpi A (1997) Mercury from combustion sources: a review of the chemical species emitted and their transport in the atmosphere. Water Air Soil Pollut 98(3-4):241–254. https://doi.org/10.1007/BF02047037
Daneshvar N, Behnajady MA, Asghar YZ (2007) Photooxidative degradation of 4-nitrophenol (4-NP) in UV/H2O2 process: influence of operational parameters and reaction mechanism. J Hazard Mater 139(2):275–279. https://doi.org/10.1016/j.jhazmat.2006.06.045
Fan HJ, Huang ST, Chung WH, Jan JL, Lin WY, Chen CC (2009) Degradation pathways of crystal violet by Fenton and Fenton-like systems: condition optimization and intermediate separation and identification. J Hazard Mater 171(1-3):1032–1044. https://doi.org/10.1016/j.jhazmat.2009.06.117
Fang P, Cen CP, Wang XM, Tang ZJ, Tang ZX, Chen DS (2013) Simultaneous removal of SO2, NO and Hg0 by wet scrubbing using urea+KMnO4 solution. Fuel Process Technol 106:645–653. https://doi.org/10.1016/j.fuproc.2012.09.060
Gogate PR, Pandit AB (2004) A view of imperative technologies for wastewater treatment: oxidation technologies at ambient conditions. Adv Environ Res 8(3-4):501–551. https://doi.org/10.1016/S1093-0191(03)00032-7
Granite EJ, King WP, Stanko DC, Pennline HW (2008) Implications of mercury interactions with band-gap semiconductor oxides. Main group. Chemistry 7:227–237
Guo RT, Pan WG, Zhang XB, Ren JX, Jin Q, Xu HJ, Wu J (2011) Removal of NO by using Fenton reagent solution in a lab-scale bubbling reactor. Fuel 90(11):3295–3298. https://doi.org/10.1016/j.fuel.2011.06.030
Han Y, Fan M, Russell AG (2015) New insights into synergistic effects and active species toward Hg0 emission control by Fe(VI) absorbent. Fuel 140:309–316. https://doi.org/10.1016/j.fuel.2014.09.072
Hanna LW, Christian TO, Klaus K, Holger VL, Torsten CS (2017) Investigation of the iron-peroxo-complex in the Fenton reaction: kinetic indication, decay kinetics and hydroxyl radical yields. Environ Sci Technol. https://doi.org/10.1021/acs.est.7b03706
Hou W, Zhou J, Qi P, Gao X, Luo Z (2014) Effect of H2S/HCl on the removal of elemental mercury in syngas over CeO2-TiO2. Chem Eng J 241:131–137. https://doi.org/10.1016/j.cej.2013.12.047
Hsueh CL, Huang YH, Wang CC, Chen CY (2005) Degradation of azo dyes using low iron concentration of Fenton and Fenton-like system. Chemosphere 58(10):1409–1414. https://doi.org/10.1016/j.chemosphere.2004.09.091
Hu Q, Zhang C, Wang Z, Yan C, Mao K, Zhang X, Xiong Y, Zhu M (2008) Photodegradation of methyl tert-butyl ether (MTBE) by UV/H2O2 and UV/TiO2. J Hazard Mater 154(1-3):795–803. https://doi.org/10.1016/j.jhazmat.2007.10.118
Kang SF, Liao CH, Chen MC (2002) Pre-oxidation and coagulation of textile wastewater by the Fenton process. Chemosphere 46(6):923–928. https://doi.org/10.1016/S0045-6535(01)00159-X
Kirby T (2013) UN agrees new treaty to reduce harm from mercury. Lancet 381(9864):362. https://doi.org/10.1016/S0140-6736(13)60153-1
Lester Y, Avisar D, Mamane H (2010) Photodegradation of the antibiotic sulphamethoxazole in water with UV/H2O2 advanced oxidation process. Environ Technol 31(2):175–183. https://doi.org/10.1080/09593330903414238
Li P, Feng XB, Qiu GL, Shang LH, Li ZG (2009a) Mercury pollution in Asia: a review of the contaminated sites. J Hazard Mater 168(2-3):591–601. https://doi.org/10.1016/j.jhazmat.2009.03.031
Li R, Yang C, Chen H, Zeng G, Yu G, Guo J (2009b) Removal of triazophos pesticide from wastewater with Fenton reagent. J Hazard Mater 167(1-3):1028–1032. https://doi.org/10.1016/j.jhazmat.2009.01.090
Li H, Ying L, CY W, Zhang J (2011) Oxidation and capture of elemental mercury over SiO2–TiO2–V2O catalysts in simulated low-rank coal combustion flue gas. Chem Eng J 169(1-3):186–193. https://doi.org/10.1016/j.cej.2011.03.003
Li H, Wu CY, Li Y, Zhang J (2012) Superior activity of MNOx-CeO2/TiO2 catalyst for catalytic oxidation of elemental mercury at low flue gas temperatures. Appl Catal B Environ 111-112:381–388. https://doi.org/10.1016/j.apcatb.2011.10.021
Liu YX, Adewuyi YG (2016) A review on removal of elemental mercury from flue gas using advanced oxidation process: chemistry and process. Chem Eng Res Des 112:199–250. https://doi.org/10.1016/j.cherd.2016.06.024
Liu YX, Wang Q (2014) Removal of elemental mercury from flue gas by thermally activated ammonium persulfate in a bubble column reactor. Environ Sci Technol 20:12181–12189
Liu YX, Zhang J (2011) Photochemical oxidation removal of NO and SO2 from simulated flue gas of Coal-Fired Power Plants by wet scrubbing using UV/H2O2 advanced oxidation process. Ind Eng Chem Res 50(7):3836–3841. https://doi.org/10.1021/ie1020377
Liu Y, Zhang J, Sheng C, Zhang Y, Zhao L (2010a) Preliminary study on a new technique for wet removal of nitric oxide from simulated flue gas with an ultraviolet (UV)/H2O2 process. Energy Fuel 24(9):4925–4930. https://doi.org/10.1021/ef1006325
Liu Y, Zhang J, Sheng C, Zhang Y, Zhao L (2010b) Simultaneous removal of NO and SO2 from coal-fired flue gas by UV/H2O2 advanced oxidation process. Chem Eng J 162(3):1006–1011. https://doi.org/10.1016/j.cej.2010.07.009
Liu YX, Zhang J, Sheng CD, Zhang YC, Zhao L (2010c) Experimental research on influencing factors of wet removal of NO from coal-fired flue gas by UV/H2O2 advanced oxidation process. Science China Technol Sci 53(7):1839–1846. https://doi.org/10.1007/s11431-010-3179-1
Liu Y, Zhang J, Pan J, Tang A (2012) Investigation on removal of NO from SO2-containing simulated flue gas by UV/Fenton-like reaction. Energy Fuel 26(9):5430–5436. https://doi.org/10.1021/ef3008568
Liu Y, Pan J, Wang Q (2014a) Removal of Hg0 from containing-SO2/NO flue gas by ultraviolet/H2O2 process in a novel photochemical reactor. AICHE J 60(6):2275–2285. https://doi.org/10.1002/aic.14388
Liu YX, Zhang J, Pan JF (2014b) Photochemical oxidation removal of Hg0 from flue gas containing SO2/NO by an ultraviolet irradiation/hydrogen peroxide (UV/H2O2) process. Energy Fuel 28(3):2135–2143. https://doi.org/10.1021/ef401697y
Liu Y, Zhang J, Yin Y (2014c) Study on absorption of elemental mercury from flue gas by UV/H2O2: process parameters and reaction mechanism. Chem Eng J 249:72–78. https://doi.org/10.1016/j.cej.2014.03.080
Liu Y, Zhang J, Yin Y (2015a) Removal of Hg0 from flue gas using two homogeneous photo-Fenton-like reactions. AICHE J 61(4):1322–1333. https://doi.org/10.1002/aic.14727
Liu Y, Zhou J, Zhang Y, Pan J, Wang Q, Zhang J (2015b) Removal of Hg0 and simultaneous removal of Hg0/SO2/NO in flue gas using two Fenton-like reagents in a spray reactor. Fuel 145:180–188. https://doi.org/10.1016/j.fuel.2014.12.084
Liu YX, Wang WY, Pan JF, Zhang YC, Zhou JF, Zhang (2015c) A study on removal of elemental mercury in flue gas using Fenton solution. J Hazard Mater 292:64–172
Liu YX, Liu ZY, Wang Y, Yin YS, Pan JF, Zhang J, Wang Q (2018) Simultaneous absorption of SO2 and NO from flue gas using ultrasound/Fe2+/heat coactivated persulfate system. J Hazard Mater 342:326–334. https://doi.org/10.1016/j.jhazmat.2017.08.042
Ma X (2008) Experimental study on removal mercury from flue gas by aqueous solution. North China Electric Power University Baoding China
Martinez AI, Deshpande BK (2007) Kinetic modeling of H2O2-enhanced oxidation of flue gas elemental mercury. Fuel Process Technol 88(10):982–987. https://doi.org/10.1016/j.fuproc.2007.05.009
Mason RP (2009) Mercury emission from natural processes and their importance in the global mercury cycle. Springer US 173–191 pp
McLarnon CR, Granite EJ, Pennline HW (2005) The PCO process for photochemical removal of mercury from flue gas. Fuel Process Technol 87(1):85–89. https://doi.org/10.1016/j.fuproc.2005.07.001
Modirshahla N, Behnajady MA (2006) Photooxidative degradation of malachite green (MG) by UV/H2O2: influence of operational parameters and kinetic modeling. Dyes & Pigm 70(1):54–59. https://doi.org/10.1016/j.dyepig.2005.04.012
Muruganandham M, Swaminathan M (2004) Photochemical oxidation of reactive azo dye with UV–H2O2 process. Dyes & Pigments 62(3):269–275. https://doi.org/10.1016/j.dyepig.2003.12.006
Neamtu M, Yediler A, Siminiceanu I, Kettrup A (2003) Oxidation of commercial reactive azo dye aqueous solutions by the photo-Fenton and Fenton-like processes. J Photochem Photobiol A Chem 161(1):87–93. https://doi.org/10.1016/S1010-6030(03)00270-3
Nidheesh PV, Gandhimathi R, Ramesh ST (2013) Degradation of dyes from aqueous solution by Fenton processes: a review. Environ Sci Pollut Res 20(4):2099–2132. https://doi.org/10.1007/s11356-012-1385-z
Ntampegliotis K, Riga A, Karayannis V, Bontozoglou V, Papapolymerou G (2006) Decolorization kinetics of Procion H-exl dyes from textile dyeing using Fenton-like reactions. J Hazard Mater 136(1):75–84. https://doi.org/10.1016/j.jhazmat.2005.11.016
Qu Z, Xie J, Xu H, Chen W, Yan N (2015) Regenerable sorbent with a high capacity for elemental mercury removal and recycling from the simulated flue gas at a low temperature. Energy Fuel 29(10):6187–6196. https://doi.org/10.1021/acs.energyfuels.5b00868
Rallo M, Lopez-Anton MA, Contreras ML, Maroto-Valer MM (2012) Mercury policy and regulations for coal-fired power plants. Environ Sci Pollut Res Int 19(4):1084–1096. https://doi.org/10.1007/s11356-011-0658-2
Sasmaz E, Aboud S, Wilcox J (2009) Hg binding on Pd binary alloys and overlays. J Phys Chem C 113(18):7813–7820. https://doi.org/10.1021/jp8112478
Selin NE (2009) Global biogeochemical cycling of mercury: a review. Annu Rev Environ Resour 34(1):43–63. https://doi.org/10.1146/annurev.environ.051308.084314
Shu HY, Chang MC (2005) Decolorization effects of six azo dyes by O3, UV/O3 and UV/H2O2 processes. Dyes Pigments 65(1):25–31. https://doi.org/10.1016/j.dyepig.2004.06.014
Subir M, Ariya PA, Dastoor AP (2012) A review of the sources of uncertainties in atmospheric mercury modeling II. Mercury surface and heterogeneous chemistry-a missing link. Atmos Environ 46:1–10. https://doi.org/10.1016/j.atmosenv.2011.07.047
Tian L, Li C, Li Q, Zeng G, Gao Z, Li S, Fan X (2009) Removal of elemental mercury by activated carbon impregnated with CeO2. Fuel 88(9):1687–1691. https://doi.org/10.1016/j.fuel.2009.01.022
Wang Z, Pehkonen SO (2004) Oxidation of elemental mercury by aqueous bromine: atmospheric implications. Atmos Environ 38(22):3675–3688. https://doi.org/10.1016/j.atmosenv.2004.02.059
Xing Y, Yan BJ, Lu P, Cui XX, Li LL, Wang MS (2017) Purification of Hg0 from flue gas by wet oxidation method and its mechanism: a review. Environ Sci Pollut Res. https://doi.org/10.1007/s11356-017-0480-6
Yang JP, Zhao YC, Ma SM, Zhu BB, Zhang JY, Zheng CG (2016a) Mercury removal by magnetic biochar derived from simultaneous activation and magnetization of sawdust. Environ Sci Technol 50(21):12040–14047. https://doi.org/10.1021/acs.est.6b03743
Yang JP, Zhao YC, Zhang JY, Zheng CG (2016b) Removal of elemental mercury from flue gas by recyclable CuCl2 modified magnetospheres catalyst from fly ash. Part 3. Regeneration performance in realistic flue gas atmosphere. Fuel 173:1–7. https://doi.org/10.1016/j.fuel.2015.12.077
Yang JP, Zhao YC, Zhang SB, Liu H, Chang L, Ma SM, Zhang JY, Zheng CG (2017) Mercury removal from flue gas by magnetospheres present in fly ash: role of iron species and modification by HF. Fuel Process Technol 167:263–270. https://doi.org/10.1016/j.fuproc.2017.07.016
Yi Z, Yao J, Ma XY (2012) Absorption behavior and removal of gaseous element mercury by sodium chlorite solution. J Environ Eng 138(6):620–624. https://doi.org/10.1061/(ASCE)EE.1943-7870.0000519
Yi Z, Hao R, Peng Z, Zhou S (2014) An integrative process for Hg0 removal using vaporized H2O2/Na2S2O8. Fuel 136:113–121
Yuan F, Hu C, Hu X, Qu J, Yang M (2009) Degradation of selected pharmaceuticals in aqueous solution with UV and UV/H2O2. Water Res 43(6):1766–1774. https://doi.org/10.1016/j.watres.2009.01.008
Zhang DL, Huang YP, Luo GF, Liu DF, Ma WH, Zhao JC (2006) Research progress of Fenton and photo-Fenton reaction. Environ Chem-Beijing 25:121–127
Zhang B, Zhong Z, Ding K, Yu L (2014) Photooxidative removal of Hg0 from simulated flue gas using UV/H2O2 advanced oxidation process: influence of operational parameters. Korean J Chem Eng 31(1):56–61. https://doi.org/10.1007/s11814-013-0179-4
Zhao L, Rochelle GT (1996) Hg absorption in aqueous permanganate. AICHE J 42(12):3559–3562. https://doi.org/10.1002/aic.690421227
Zhao Y, Ma X, Liu S, Yao J (2009) Experiments on and mechanism of simultaneous removal of Hg0, SO2 and NO from flus gas using NaClO2 solution. Environ Technol 30(3):277–282. https://doi.org/10.1080/09593330802573795
Zhou CS, Sun LS, Xiang J, Hu S, Su S, Zhang AC (2015a) The experimental and mechanism study of novel heterogeneous Fenton-like reactions using Fe3_xTixO4 catalysts for Hg0 absorption. Proc Combust Inst 35(3):2875–2882. https://doi.org/10.1016/j.proci.2014.06.049
Zhou CS, Sun LS, Zhang AC, Ma C, Wang B, Yu J, Su S, Hu S, Xiang J (2015b) Elemental mercury (Hg0) removal from containing SO2/NO flue gas by magnetically separable Fe2.45Ti0.55O4/H2O2 advanced oxidation processes. Chem Eng J 273:381–389. https://doi.org/10.1016/j.cej.2015.03.105
Zhou CS, Sun LS, Zhang AC, XF W, Ma C, Su S, Hu S, Xiang J (2015c) Fe3_xCuxO4 as highly active heterogeneous Fenton-like catalysts toward elemental mercury removal. Chemosphere 125:16–24. https://doi.org/10.1016/j.chemosphere.2014.12.082
Zhou CS, Wang B, Song ZJ, Ma C, Yu J, Zhang ZY, Yang HM, Sun LS (2017) DFT studies of Hg0 oxidation by gaseous advanced oxidation method: H2O2/Fe3O4 (111) and hydroxyl pre-adsorbed Fe3O4 (111) surface. Fuel 202:318–327. https://doi.org/10.1016/j.fuel.2017.04.041
Funding
This work was supported by the National Key R&D Program of China (No. 2017YFC0210301, 2017YFC0210303), Joint Funds of the National Natural Science Foundation of China (No.U1560110), Beijing Science and Technology Project (No.D161100004516001, D161100004416001), and Fundamental Research Funds for the Central Universities.
Author information
Authors and Affiliations
Corresponding authors
Additional information
Responsible editor: Vítor Pais Vilar
Rights and permissions
About this article
Cite this article
Xing, Y., Li, L., Lu, P. et al. Simultaneous purifying of Hg0, SO2, and NOx from flue gas by Fe3+/H2O2: the performance and purifying mechanism. Environ Sci Pollut Res 25, 6456–6465 (2018). https://doi.org/10.1007/s11356-017-0948-4
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-017-0948-4