Abstract
The ozone-wet absorption process has attracted widespread attention as an efficient and low-pollution approach for flue gas simultaneous desulfurization and denitrification. Key issues for ozone-wet absorption process mainly focused on how to enhance the ozonation efficiencies, which were always confined by the relatively low mass transfer because of low solubility and stability of ozone in the liquid phase. Cavitation is an effective way to reduce ozone mass transfer resistance by causing turbulence in bulk solution and microcirculation surrounding cavitation bubbles. Therefore, this study innovatively combines cavitation with the ozone-wet oxidation process and applies it for the rapid and simultaneous oxidation of NOX and SO2 from flue gases as a desulfurization and denitrification process. The system as developed was examined under different operating conditions such as system pH, sodium dodecylbenzene sulfonate (SDBS) concentration, iron (Fe2+), and manganese (Mn2+) content. All of the investigated parameters influenced NOX removal, and the SO2 removal rate was always kept high. The NOX and SO2 removal efficiency of as design process was found to be 89.2% for NOX and 98.7% for SO2 under optimum experimental conditions (i.e., 0.06 g/L of SDBS, 1.5 mmol/L of Fe2+ and pH of 12.0). The involvement of reactive ·OH was identified using tert-butanol alcohol for the oxidative removal of SO2 and NOX. The system can be used for the reduction of flue gas pollutants and environmental cleanup.
Graphical Abstract
Similar content being viewed by others
Data Availability
All data generated or analyzed during this study are included in this published article.
References
Abramov, V. O., Abramova, A. V., Cravotto, G., Nikonov, R. V., Fedulov, I. S., & Ivanov, V. K. (2021). Flow-mode water treatment under simultaneous hydrodynamic cavitation and plasma. Ultrasonics Sonochemistry, 70, 105323. https://doi.org/10.1016/j.ultsonch.2020.105323
Ahmadi, G. R., & Toghraie, D. (2016). Energy and exergy analysis of Montazeri Steam Power Plant in Iran. Renewable & Sustainable Energy Reviews, 56, 454–463. https://doi.org/10.1016/j.rser.2015.11.074
Anaokar, G. S., & Khambete, A. K. (2021). Fuzzy rule base approach to evaluate performance of hydrodynamic cavitation for borewell water softening. Materials Today: Proceedings, 47, 1377–1383. https://doi.org/10.1016/j.matpr.2021.02.404
Atwi, K., Wilson, S. N., Mondal, A., Edenfield, R. C., Crow, K. M. S., El Hajj, O., Perrie, C., Glenn, C. K., Easley, C. A., Handa, H., & Saleh, R. (2022). Differential response of human lung epithelial cells to particulate matter in fresh and photochemically aged biomass-burning smoke. Atmospheric Environment, 271, 118929. https://doi.org/10.1016/j.atmosenv.2021.118929
Bamperng, S., Suwannachart, T., Atchariyawut, S., & Jiraratananon, R. (2010). Ozonation of dye wastewater by membrane contactor using PVDF and PTFE membranes. Separation and Purification Technology, 72(2), 186–193. https://doi.org/10.1016/j.seppur.2010.02.006
Boczkaj, G., Gagol, M., Klein, M., & Przyjazny, A. (2018). Effective method of treatment of effluents from production of bitumens under basic pH conditions using hydrodynamic cavitation aided by external oxidants. Ultrasonics Sonochemistry, 40, 969–979. https://doi.org/10.1016/j.ultsonch.2017.08.032
Brijkishore, Khare, R., & Prasad, V. (2021). Prediction of cavitation and its mitigation techniques in hydraulic turbines-a review. Ocean Engineering, 221, 108512. https://doi.org/10.1016/j.oceaneng.2020.108512
Cheng, Z., Yang, R., & Wang, Y. (2017). Mn/sepiolite as the heterogeneous ozonation catalysts applied to the advanced treatment of regenerated-papermaking wastewater. Water Science and Technology, 75(5), 1025–1033. https://doi.org/10.2166/wst.2016.583
Chu, H., Chien, T. W., & Li, S. Y. (2001). Simultaneous absorption of SO2 and NO from flue gas with KMnO4/NaOH solutions. Science of the Total Environment, 275(1–3), 127–135. https://doi.org/10.1016/s0048-9697(00)00860-3
Cobra, P. F., Gomes, B. F., Nascimento Mitre, C. I., Barbosa, L. L., Marconcini, L. V., & Colnago, L. A. (2015). Measuring the solubility product constant of paramagnetic cations using time-domain nuclear magnetic resonance relaxometry. Microchemical Journal, 121, 14–17. https://doi.org/10.1016/j.microc.2015.02.002
Cordoba, P. (2015). Status of flue gas desulphurisation (FGD) systems from coal-fired power plants: Overview of the physic-chemical control processes of wet limestone FGDs. Fuel, 144, 274–286. https://doi.org/10.1016/j.fuel.2014.12.065
Dong, Y., Yuan, H., Bai, L., Ge, D., & Zhu, N. (2022). A comprehensive study on simultaneous enhancement of sludge dewaterability and elimination of polycyclic aromatic hydrocarbons by Fe2+ catalyzing O-3 process. Science of the Total Environment, 819, 152015. https://doi.org/10.1016/j.scitotenv.2021.152015
Fedorov, K., Sun, X., & Boczkaj, G. (2021). Combination of hydrodynamic cavitation and SR-AOPs for simultaneous degradation of BTEX in water. Chemical Engineering Journal, 417, 128081. https://doi.org/10.1016/j.cej.2020.128081
Fischbacher, A., von Sonntag, C., & Schmidt, T. C. (2017). Hydroxyl radical yields in the Fenton process under various pH, ligand concentrations and hydrogen peroxide/Fe(II) ratios. Chemosphere, 182, 738–744. https://doi.org/10.1016/j.chemosphere.2017.05.039
Ge, M., Petkovsek, M., Zhang, G., Jacobs, D., & Coutier-Delgosha, O. (2021). Cavitation dynamics and thermodynamic effects at elevated temperatures in a small Venturi channel. International Journal of Heat and Mass Transfer, 170, 120970. https://doi.org/10.1016/j.ijheatmasstransfer.2021.120970
Gogate, P. R., Mededovic-Thagard, S., McGuire, D., Chapas, G., Blackmon, J., & Cathey, R. (2014). Hybrid reactor based on combined cavitation and ozonation: From concept to practical reality. Ultrasonics Sonochemistry, 21(2), 590–598. https://doi.org/10.1016/j.ultsonch.2013.08.016
Hao, R., Wang, X., Zhao, X., Xu, M., Zhao, Y., Mao, X., Yuan, B., Zhang, Y., & Gao, K. (2018). A novel integrated method of vapor oxidation with dual absorption for simultaneous removal of SO2 and NO: Feasibility and prospect. Chemical Engineering Journal, 333, 583–593. https://doi.org/10.1016/j.cej.2017.09.191
Hollender, J., Zimmermann, S. G., Koepke, S., Krauss, M., McArdell, C. S., Ort, C., Singer, H., von Gunten, U., & Siegrist, H. (2009). Elimination of organic micropollutants in a municipal wastewater treatment plant upgraded with a full-scale post-ozonation followed by sand filtration. Environmental Science & Technology, 43(20), 7862–7869. https://doi.org/10.1021/es9014629
Hulten, A. H., Nilsson, P., Samuelsson, M., Ajdari, S., Normann, F., & Andersson, K. (2017). First evaluation of a multicomponent flue gas cleaning concept using chlorine dioxide gas - experiments on chemistry and process performance. Fuel, 210, 885–891. https://doi.org/10.1016/j.fuel.2017.08.116
Kang, M. S., Shin, J., Yu, T. U., & Hwang, J. (2020). Simultaneous removal of gaseous NOx and SO2 by gas-phase oxidation with ozone and wet scrubbing with sodium hydroxide. Chemical Engineering Journal, 381, 122601. https://doi.org/10.1016/j.cej.2019.122601
Laipan, M., Fu, H., Zhu, R., Sun, L., Zhu, J., & He, H. (2017). Converting spent Cu/Fe layered double hydroxide into Cr(VI) reductant and porous carbon material. Scientific Reports, 7, 7277. https://doi.org/10.1038/s41598-017-07775-8
Li, H. Y., Qu, J. H., Zhao, X., & Liu, H. J. (2004). Removal of alachlor from water by catalyzed ozonation in the presence of Fe2+, Mn2+, and humic substances. Journal of Environmental Science and Health Part B-Pesticides Food Contaminants and Agricultural Wastes, 39(5–6), 791–803. https://doi.org/10.1081/lesb-200030870
Li, D., Xiao, Z., Bin Aftab, T., & Xu, S. (2018). Flue gas denitration by wet oxidation absorption methods: Current status and development. Environmental Engineering Science, 35(11), 1151–1164. https://doi.org/10.1089/ees.2017.0516
Li, H., Liu, J., Chen, S., & Lv, W. (2022). Numerical investigation of ozone decomposition by self-excited oscillation cavitation jet. Open Physics, 20(1), 94–105. https://doi.org/10.1515/phys-2022-0005
Liu, Y., Wang, Q., Yin, Y., Pan, J., & Zhang, J. (2014). Advanced oxidation removal of NO and SO2 from flue gas by using ultraviolet/H2O2/NaOH process. Chemical Engineering Research & Design, 92(10), 1907–1914. https://doi.org/10.1016/j.cherd.2013.12.015
Liu, Y., Wang, Y., Xu, W., Yang, W., Pan, Z., & Wang, Q. (2018). Simultaneous absorption-oxidation of nitric oxide and sulfur dioxide using ammonium persulfate synergistically activated by UV-light and heat. Chemical Engineering Research & Design, 130, 321–333. https://doi.org/10.1016/j.cherd.2017.12.043
Luo, C., Gu, J., Tong, Z., Chen, L., Zhou, W., Wu, K., & Ren, X. (2021). Dynamics of laser-induced cavitation bubbles near a short hole and laser cavitation processing with particles. Optics and Laser Technology, 135, 106680. https://doi.org/10.1016/j.optlastec.2020.106680
McClure, D. D., Deligny, J., Kavanagh, J. M., Barton, G. W., & Fletcher, D. F. (2012). The effect of surfactant addition on hold-up, bubble size and mixing time in bubble column reactors. New Biotechnology, 29, S11–S12. https://doi.org/10.1016/j.nbt.2012.08.023
Nawaz, F., Khan, B. U., Ullah, H., Islam, Z. U., Khan, G. U., Khayam, M., Waseem, M., Khan, G., & Khan, M. A. (2021). Efficient hydroxyl radical production with Sodium salts of surfactants ozonation for treatment of organic acid pollutants in wastewater. Environmental Technology & Innovation, 22, 101451. https://doi.org/10.1016/j.eti.2021.101451
Nishiyama, T., Matsuura, K., Sato, E., Kometani, N., & Horibe, H. (2017). Degradation of hydrophilic polymers in aqueous solution by using ozone microbubble. Journal of Photopolymer Science and Technology, 30(3), 285–289. https://doi.org/10.2494/photopolymer.30.285
Ouederni, A., Mora, J. C., & Bes, R. S. (1987). Ozone absorption in water - mass-transfer and solubility. Ozone-Science & Engineering, 9(1), 1–12. https://doi.org/10.1080/01919518708552384
Park, J.-H., Ahn, J.-W., Kim, K.-H., & Son, Y.-S. (2019). Historic and futuristic review of electron beam technology for the treatment of SO2 and NOx in flue gas. Chemical Engineering Journal, 355, 351–366. https://doi.org/10.1016/j.cej.2018.08.103
Pazheri, F. R., Othman, M. F., & Malik, N. H. (2014). A review on global renewable electricity scenario. Renewable & Sustainable Energy Reviews, 31, 835–845. https://doi.org/10.1016/j.rser.2013.12.020
Qiao, X., Du, J., Kota, S. H., Ying, Q., Xiao, W., & Tang, Y. (2018). Wet deposition of sulfur and nitrogen in Jiuzhaigou National Nature Reserve, Sichuan, China during 2015–2016: Possible effects from regional emission reduction and local tourist activities. Environmental Pollution, 233, 267–277. https://doi.org/10.1016/j.envpol.2017.08.041
Raghunath, C. V., & Mondal, M. K. (2017). Experimental scale multi component absorption of SO2 and NO by NH3/NaClO scrubbing. Chemical Engineering Journal, 314, 537–547. https://doi.org/10.1016/j.cej.2016.12.011
Rigby, M., Park, S., Saito, T., Western, L. M., Redington, A. L., Fang, X., Henne, S., Manning, A. J., Prinn, R. G., Dutton, G. S., Fraser, P. J., Ganesan, A. L., Hall, B. D., Harth, C. M., Kim, J., Kim, K. R., Krummel, P. B., Lee, T., Li, S., . . . Young, D. (2019). Increase in CFC-11 emissions from eastern China based on atmospheric observations. Nature, 569(7757), 546-+. https://doi.org/10.1038/s41586-019-1193-4
Satoh, A. Y., Trosko, J. E., & Masten, S. J. (2007). Methylene blue dye test for rapid qualitative detection of hydroxyl radicals formed in a Fenton’s reaction aqueous solution. Environmental Science & Technology, 41(8), 2881–2887. https://doi.org/10.1021/es0617800
Sauleda, R., & Brillas, E. (2001). Mineralization of aniline and 4-chlorophenol in acidic solution by ozonation catalyzed with Fe2+ and UVA light. Applied Catalysis B-Environmental, 29(2), 135–145. https://doi.org/10.1016/s0926-3373(00)00197-1
Sun, W.-Y., Ding, S.-L., Zeng, S.-S., Su, S.-J., & Jiang, W.-J. (2011). Simultaneous absorption of NOx and SO2 from flue gas with pyrolusite slurry combined with gas-phase oxidation of NO using ozone. Journal of Hazardous Materials, 192(1), 124–130. https://doi.org/10.1016/j.jhazmat.2011.04.104
Sun, C., Zhao, N., Zhuang, Z., Wang, H., Liu, Y., Weng, X., & Wu, Z. (2014). Mechanisms and reaction pathways for simultaneous oxidation of NOx and SO2 by ozone determined by in situ IR measurements. Journal of Hazardous Materials, 274, 376–383. https://doi.org/10.1016/j.jhazmat.2014.04.027
Sun, X., Xuan, X., Ji, L., Chen, S., Liu, J., Zhao, S., Park, S., Yoon, J. Y., & Om, A. S. (2021). A novel continuous hydrodynamic cavitation technology for the inactivation of pathogens in milk. Ultrasonics Sonochemistry, 71, 105382. https://doi.org/10.1016/j.ultsonch.2020.105382
Wang, B., Xiong, X., Shui, Y., Huang, Z., & Tian, K. (2019a). A systematic study of enhanced ozone mass transfer for ultrasonic-assisted PTFE hollow fiber membrane aeration process. Chemical Engineering Journal, 357, 678–688. https://doi.org/10.1016/j.cej.2018.09.188
Wang, H., Yuan, B., Hao, R., Zhao, Y., & Wang, X. (2019). A critical review on the method of simultaneous removal of multi-air-pollutant in flue gas. Chemical Engineering Journal, 378, 122155. https://doi.org/10.1016/j.cej.2019.122155
Wang, J., Chen, H., Yuan, R., Wang, F., Ma, F., & Zhou, B. (2020). Intensified degradation of textile wastewater using a novel treatment of hydrodynamic cavitation with the combination of ozone. Journal of Environmental Chemical Engineering, 8(4), 103959. https://doi.org/10.1016/j.jece.2020.103959
Wang, T., Song, Y., Ding, H., Liu, Z., Baldwin, A., Wong, I., Li, H., & Zhao, C. (2020). Insight into synergies between ozone and in-situ regenerated granular activated carbon particle electrodes in a three-dimensional electrochemical reactor for highly efficient nitrobenzene degradation. Chemical Engineering Journal, 394, 124852. https://doi.org/10.1016/j.cej.2020.124852
Wang, Y., Han, X., Chen, M., Cui, S., Ma, X., & Hao, L. (2021). Desulfurization and denitrification performance of modified rice husk ash-carbide slag absorbent. Materials, 14(1), 68. https://doi.org/10.3390/ma14010068
Wu, J., Zhang, K., Cen, C., Wu, X., Mao, R., & Zheng, Y. (2021). Role of bulk nanobubbles in removing organic pollutants in wastewater treatment. AMB Express, 11(1), 96. https://doi.org/10.1186/s13568-021-01254-0
Xiao, Z., Li, D., Zhu, Q., & Sun, Z. (2020). Simultaneous removal of NO and SO2 through a new wet recycling oxidation-reduction process utilizing micro-nano bubble gas-liquid dispersion system based on Na2SO3. Fuel, 263, 116682. https://doi.org/10.1016/j.fuel.2019.116682
Zhang, Q., Dong, Z., Zhao, S., Liu, Z., & Chen, G. (2021). Ultrasound-assisted gas-liquid mass transfer process in microreactors: the influence of surfactant, channel size and ultrasound frequency. Chemical Engineering Journal, 405, 126720. https://doi.org/10.1016/j.cej.2020.126720
Funding
Support provided by the Natural Science Foundation of China-Joint Fund for Steel (U1660107).
Author information
Authors and Affiliations
Contributions
Fan Zhang: writing — original draft, visualization. Asif Hussain: grammar check and writing manuscript. Jingyi Ma: conceptualization, methodology, supervision. Xi Wang: data analysis and writing manuscript. Xing Wang: data analysis and writing manuscript. Yuanyuan Guo: software. Shihong Xu: formulation of idea and review/editing. Dengxin Li: formulation of idea and review/editing.
Corresponding authors
Ethics declarations
Consent to Participate
All the people involved in this work gave their consent to participate.
Consent for Publication
All the authors have given their consent for the publication of the study.
Competing Interests
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Zhang, F., Hussain, A., Ma, J. et al. Simultaneous Oxidation of SO2 and NOX via Hydroxyl Radicals Using Ozone-Cavitation-Absorption System. Water Air Soil Pollut 234, 165 (2023). https://doi.org/10.1007/s11270-022-06034-5
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-022-06034-5