Integrative Process for Simultaneous Removal of SO2 and NO Utilizing a Vaporized H2O2/Na2S2O8

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School of Environmental Science & Engineering, North China Electric Power University, 071003 Baoding, Hebei Province People’s Republic of China
Cite this: Energy Fuels 2014, 28, 10, 6502–6510
Publication Date (Web):September 8, 2014
https://doi.org/10.1021/ef501686j
Copyright © 2014 American Chemical Society
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Abstract

A novel integrative process for simultaneous removal of SO2 and NO from coal-fired flue gas was designed, in which, SO2 and NO were initially oxidized by a vaporized complex oxidant composed of hydrogen peroxide (H2O2) and sodium persulfate (Na2S2O8) (HN solution) and then absorbed by the Ca(OH)2 that followed. The effects of various reaction factors on the simultaneous removal were investigated, such as the concentration of Na2S2O8, the transition metal additives, the HN pH, the adding rate of HN, the residence time of flue gas, the reaction temperature, and the concentrations of coexistence gases O2, SO2, NO, and CO2. Under the optimal conditions, the simultaneous removal efficiencies of 98.9% for SO2 and 79.6% for NO were obtained. The reaction mechanism was speculated based on the characterization of removal products by scanning electron microscopy and X-ray diffraction and related literature references. Meanwhile, the macrokinetics of desulfurization and denitrification were also calculated.

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  3. Yan Wang, Yong Wang, Yangxian Liu. Absorption of H2S from Gas Streams by the Wet Ultraviolet/Persulfate Oxidation Process: Mechanism and Kinetics. Energy & Fuels 2020, 34 (7) , 8037-8045. https://doi.org/10.1021/acs.energyfuels.0c00755
  4. Yu-Xuan Li, Rui-Tang Guo, Zhong-Yi Wang, Xu Shi, Wei-Guo Pan. Removal of NO by Using Sodium Persulfate Solution: Catalyzed by Different Nanostructured MnO2. Energy & Fuels 2020, 34 (3) , 3477-3482. https://doi.org/10.1021/acs.energyfuels.9b03856
  5. Hongyuan Xi, Song Zhou, Zhao Zhang. Novel Method Using Na2S2O8 as an Oxidant to Simultaneously Absorb SO2 and NO from Marine Diesel Engine Exhaust Gases. Energy & Fuels 2020, 34 (2) , 1984-1991. https://doi.org/10.1021/acs.energyfuels.9b03334
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  7. Shujun Sun, Suxia Ma, Bingchuan Yang, Rongji Cui, Jie Wang. NO Removal from Flue Gas by Using Chlorine Dioxide Solution. Energy & Fuels 2019, 33 (10) , 10004-10010. https://doi.org/10.1021/acs.energyfuels.9b01694
  8. Wenxia Xie, Chengwei Xu, Jun Zhang, Yangxian Liu, Jianfei Xi, Jianhong Lv, Zhongzhu Gu. Simultaneous Removal of SO2 and NO Using H2O2/Urea Activated by Vacuum Ultraviolet Light in a Pilot-Scale Spraying Tower. Energy & Fuels 2019, 33 (2) , 1325-1333. https://doi.org/10.1021/acs.energyfuels.8b03154
  9. Ziheng Meng, Chenye Wang, Xingrui Wang, Yan Chen, and Huiquan Li . Simultaneous Removal of SO2 and NOx from Coal-Fired Flue Gas Using Steel Slag Slurry. Energy & Fuels 2018, 32 (2) , 2028-2036. https://doi.org/10.1021/acs.energyfuels.7b03385
  10. Yi Zhao, Wen Qiu, Chunyan Yang, and Jianan Wang . Study on a Novel Oxidation Process for Removing Arsenic from Flue Gas. Energy & Fuels 2017, 31 (1) , 693-698. https://doi.org/10.1021/acs.energyfuels.6b01724
  11. Hyung Jun Yoon, Hyun-Woo Park, and Dong-Wha Park . Simultaneous Oxidation and Absorption of NOx and SO2 in an Integrated O3 Oxidation/Wet Atomizing System. Energy & Fuels 2016, 30 (4) , 3289-3297. https://doi.org/10.1021/acs.energyfuels.5b02924
  12. Runlong Hao and Yi Zhao . Macrokinetics of NO Oxidation by Vaporized H2O2 Association with Ultraviolet Light. Energy & Fuels 2016, 30 (3) , 2365-2372. https://doi.org/10.1021/acs.energyfuels.5b02748
  13. Zhiping Wang and Zuwu Wang . Mass Transfer-Reaction Kinetics Study on Absorption of NO with Dual Oxidants (H2O2/S2O82–). Industrial & Engineering Chemistry Research 2015, 54 (41) , 9905-9912. https://doi.org/10.1021/acs.iecr.5b02162
  14. Yeawan Lee, Jin-Ho Sung, Bangwoo Han, Yong-Jin Kim, Hak-Joon Kim. Minimizing the consumption of reducing agents for NOx removal in a wet scrubber without H2S formation. Separation and Purification Technology 2021, 31 , 120101. https://doi.org/10.1016/j.seppur.2021.120101
  15. Feng Shi, Kan Li, Juexiu Li, Diwen Ying, Jinping Jia, Tonghua Sun, Naiqiang Yan, Xiaojing Zhang. Simultaneous wet absorption of SO2 and NOX with mixed Na2SO3 and (NH4)2SO3: Effects of mass concentration ratio and pH. Chemical Engineering Journal 2021, 421 , 129945. https://doi.org/10.1016/j.cej.2021.129945
  16. Xuan Liu, Chang’an Wang, Tao Zhu, Qiang Lv, Defu Che. Simultaneous removal of SO2 and NO with OH from the catalytic decomposition of H2O2 over Fe-Mo mixed oxides. Journal of Hazardous Materials 2021, 404 , 123936. https://doi.org/10.1016/j.jhazmat.2020.123936
  17. Yang Li, Defu Che, Chenglong Yang, Mingyu Yao, Tingwen Zhao, Kangli Fu, Hanchen Zhao. Engineering practice and economic analysis of ozone oxidation wet denitrification technology. Chinese Journal of Chemical Engineering 2021, 29 , 401-408. https://doi.org/10.1016/j.cjche.2020.08.042
  18. Runlong Hao, Yichen Luo, Zhen Qian, Zhao Ma, Yuqiao Ding, Yaping Gong, Zheng Wang, Yi Zhao. Simultaneous removal of SO2, NO and Hg0 using an enhanced gas phase UV-AOP method. Science of The Total Environment 2020, 734 , 139266. https://doi.org/10.1016/j.scitotenv.2020.139266
  19. Yan Wang, Yangxian Liu, Shuo Shi. Removal of nitric oxide from flue gas using novel microwave-activated double oxidants system. Chemical Engineering Journal 2020, 393 , 124754. https://doi.org/10.1016/j.cej.2020.124754
  20. Runlong Hao, Chu Li, Zheng Wang, Yaping Gong, Bo Yuan, Yi Zhao, Lidong Wang, John Crittenden. Removal of gaseous elemental mercury using thermally catalytic chlorite-persulfate complex. Chemical Engineering Journal 2020, 391 , 123508. https://doi.org/10.1016/j.cej.2019.123508
  21. Yang Li, Defu Che, Hanchen Zhao, Chenglong Yang, Tingwen Zhao, Guangwen Cheng, Mingyu Yao. Tributyl phosphate additive enhancing catalytic absorption of NO2 for simultaneous removal of SO2/NOx in wet desulfurization system. Journal of the Energy Institute 2020, 93 (2) , 474-481. https://doi.org/10.1016/j.joei.2019.07.004
  22. Xincheng Wang, Xiangjun Zhang, Minyao He, Yongji Song, Cuiqing Li, Hong Wang. Promoting effect of multi-transition metals on the NO reduction by NH3 over TiO2 catalyst studied with in situ DRIFTS. Research on Chemical Intermediates 2020, 46 (3) , 1663-1684. https://doi.org/10.1007/s11164-019-04055-0
  23. Bo Yuan, Yi Zhao, Xingzhou Mao, Zehui Zheng, Runlong Hao. Simultaneous removal of SO2, NO and Hg0 from flue gas using vaporized oxidant catalyzed by Fe/ZSM-5. Fuel 2020, 262 , 116567. https://doi.org/10.1016/j.fuel.2019.116567
  24. Runlong Hao, Zheng Wang, Yaping Gong, Zhao Ma, Zhen Qian, Yichen Luo, Bo Yuan, Yi Zhao. Photocatalytic removal of NO and Hg0 using microwave induced ultraviolet irradiating H2O/O2 mixture. Journal of Hazardous Materials 2020, 383 , 121135. https://doi.org/10.1016/j.jhazmat.2019.121135
  25. Bo Yuan, Xingzhou Mao, Zheng Wang, Runlong Hao, Yi Zhao. Radical-induced oxidation removal of multi-air-pollutant: A critical review. Journal of Hazardous Materials 2020, 383 , 121162. https://doi.org/10.1016/j.jhazmat.2019.121162
  26. Chunlai Liu, Jing Li, Changlin Yang, Zhenheng Diao, Chengxue Wang. A composite absorption liquid for simultaneous desulfurization and denitrification in flue gas. Chinese Journal of Chemical Engineering 2019, 27 (10) , 2566-2573. https://doi.org/10.1016/j.cjche.2019.04.013
  27. Masoumeh Moheb Shahrestani, Amir Rahimi. Evaluation of electrical energy consumption in UV/H2O2 advanced oxidation process for simultaneous removal of NO and SO2. Environmental Engineering Research 2019, 24 (3) , 389-396. https://doi.org/10.4491/eer.2018.276
  28. Xuan Liu, Chang'an Wang, Tao Zhu, Qiang Lv, Yang Li, Defu Che. Simultaneous removal of NO and SO2 from coal-fired flue gas based on the catalytic decomposition of H2O2 over Fe2(MoO4)3. Chemical Engineering Journal 2019, 371 , 486-499. https://doi.org/10.1016/j.cej.2019.04.028
  29. Jiaqi Wei, Junjie Gu, Junheng Guo, Wei Li, Chenglong Wang, Jinli Zhang. Simultaneous removal of nitrogen oxides and sulfur dioxide using ultrasonically atomized hydrogen peroxide. Environmental Science and Pollution Research 2019, 26 (22) , 22351-22361. https://doi.org/10.1007/s11356-019-05531-1
  30. Yongji Song, Ting Wang, Liang Cheng, Cuiqing Li, Hong Wang, Xincheng Wang. Simultaneous removal of SO 2 and NO by CO reduction over prevulcanized Fe 2 O 3 /AC catalysts. The Canadian Journal of Chemical Engineering 2019, 97 (7) , 2015-2020. https://doi.org/10.1002/cjce.23439
  31. Wenxia Xie, Chengwei Xu, Jun Zhang, Yangxian Liu, Jianfei Xi, Zhongzhu Gu, Jianhong Lv. Effects of experimental parameters on simultaneous removal of SO 2 and NO by VUV/H 2 O 2 advanced oxidation process in a pilot-scale photochemical spraying tower. Journal of Chemical Technology & Biotechnology 2019, 94 (3) , 721-729. https://doi.org/10.1002/jctb.5816
  32. Zean Wang, Hu Jin, Kun Wang, Yihao Xie, Jian Ning, Yaojie Tu, Yingming Chen, Hao Liu, Hancai Zeng. A two-step method for the integrated removal of HCl, SO2 and NO at low temperature using viscose-based activated carbon fibers modified by nitric acid. Fuel 2019, 239 , 272-281. https://doi.org/10.1016/j.fuel.2018.11.002
  33. Myung Soo Kang, Jungho Hwang. Effect of SO2 Concentration on NOx Removal Efficiency in NaOH-Based Wet Scrubbing. Journal of Korean Society for Atmospheric Environment 2018, 34 (5) , 659-667. https://doi.org/10.5572/KOSAE.2018.34.5.659
  34. Xue Kang, Xiaoxun Ma, Jian'an Yin, Xuchun Gao. A study on simultaneous removal of NO and SO 2 by using sodium persulfate aqueous scrubbing. Chinese Journal of Chemical Engineering 2018, 26 (7) , 1536-1544. https://doi.org/10.1016/j.cjche.2018.02.026
  35. Bal Raj Deshwal, Neha Kundu. Comparing Acidic Sodium Hypochlorite and Sodium Chlorite Solutions for Controlling Nitrogen Oxides Emission. Environmental Engineering Science 2018, 35 (5) , 430-436. https://doi.org/10.1089/ees.2017.0262
  36. Zhitao Han, Dongsheng Zhao, Dekang Zheng, Xinxiang Pan, Bojun Liu, Zhiwei Han, Yu Gao, Junming Wang, Zhijun Yan. NO Removal from Simulated Flue Gas with a NaClO2 Mist Generated Using the Ultrasonic Atomization Method. Energies 2018, 11 (5) , 1043. https://doi.org/10.3390/en11051043
  37. Haiqian Zhao, Xingcun Gao, Chenghao Liu, Zhonghua Wang, Hanbing Qi. Basic rules of NO oxidation by Fe 2+ /H 2 O 2 /AA directional decomposition system. The Canadian Journal of Chemical Engineering 2018, 96 (1) , 27-32. https://doi.org/10.1002/cjce.22888
  38. Yi Zhao, Wen Qiu. Arsenic oxidation and removal from flue gas using H2O2/Na2S2O8 solution. Fuel Processing Technology 2017, 167 , 355-362. https://doi.org/10.1016/j.fuproc.2017.07.021
  39. Wei Yang, Yangxian Liu, Wen Xu, Qian Wang, Liang Zhao, Jianfeng Pan. Oxidation-separation kinetics of nitric oxide from flue gas using ferrate (VI) reagent in a spraying reactor. The Canadian Journal of Chemical Engineering 2017, 95 (7) , 1364-1372. https://doi.org/10.1002/cjce.22778
  40. Runlong Hao, Shuo Yang, Yi Zhao, Yaoyu Zhang, Bo Yuan, Xingzhou Mao. Follow-up research of ultraviolet catalyzing vaporized H 2 O 2 for simultaneous removal of SO 2 and NO: Absorption of NO 2 and NO by Na-based WFGD byproduct (Na 2 SO 3 ). Fuel Processing Technology 2017, 160 , 64-69. https://doi.org/10.1016/j.fuproc.2017.02.021
  41. Runlong Hao, Shuo Yang, Bo Yuan, Yi Zhao. Simultaneous desulfurization and denitrification through an integrative process utilizing NaClO 2 /Na 2 S 2 O 8. Fuel Processing Technology 2017, 159 , 145-152. https://doi.org/10.1016/j.fuproc.2017.01.018
  42. Yi Zhao, Runlong Hao, Fangming Xue, Yanan Feng. Simultaneous removal of multi-pollutants from flue gas by a vaporized composite absorbent. Journal of Hazardous Materials 2017, 321 , 500-508. https://doi.org/10.1016/j.jhazmat.2016.09.044
  43. Zhitao Han, Shaolong Yang, Dongsheng Zhao, Bojun Liu, Xinxiang Pan, Zhijun Yan. An investigation of mass transfer-reaction kinetics of NO absorption by wet scrubbing using an electrolyzed seawater solution. RSC Advances 2017, 7 (31) , 18821-18829. https://doi.org/10.1039/C7RA01608E
  44. Bo Wu, Yuanquan Xiong, Jinbo Ru, Hao Feng. Enhancement of NO absorption in ammonium-based solution using heterogeneous Fenton reaction at low H2O2 consumption. Korean Journal of Chemical Engineering 2016, 33 (12) , 3407-3416. https://doi.org/10.1007/s11814-016-0195-2
  45. Runlong Hao, Yi Zhao, Bo Yuan, Sihan Zhou, Shuo Yang. Establishment of a novel advanced oxidation process for economical and effective removal of SO2 and NO. Journal of Hazardous Materials 2016, 318 , 224-232. https://doi.org/10.1016/j.jhazmat.2016.06.052
  46. Zhiping Wang, Zuwu Wang. Reaction performance study on denitration in aqueous solution of the dual oxidant (H 2 O 2 /S 2 O82−). Environmental Progress & Sustainable Energy 2016, 35 (5) , 1361-1366. https://doi.org/10.1002/ep.12359
  47. Wenkai Zhao, Qin Zhong, Jie Ding, Zhiyong Deng, Lina Guo, Fujiao Song. Enhanced catalytic ozonation over reduced spinel CoMn 2 O 4 for NO x removal: active site and mechanism analysis. RSC Advances 2016, 6 (116) , 115213-115221. https://doi.org/10.1039/C6RA21544K
  48. Yi Zhao, Runlong Hao, Tianhao Wang, Chunyan Yang. Follow-up research for integrative process of pre-oxidation and post-absorption cleaning flue gas: Absorption of NO2, NO and SO2. Chemical Engineering Journal 2015, 273 , 55-65. https://doi.org/10.1016/j.cej.2015.03.053