Citation: CHI Gui-long, SHEN Bo-xiong, ZHU Shao-wen, HE Chuan. Oxidation of elemental mercury over modified SCR catalysts[J]. Journal of Fuel Chemistry and Technology, ;2016, 44(6): 763-768. shu

Oxidation of elemental mercury over modified SCR catalysts

1.
College of Environmental Science and Engineering, Nankai University, Tianjin 300071, China
2.
College of Energy and Environmental Engineering, Hebei University of Technology, Tianjin 300401, China

Corresponding author: SHEN Bo-xiong, shenboxiong0722@sina.com
Received Date: 12 January 2016
Revised Date: 17 March 2016

Figures(6)

The oxidation activity of elemental mercury (Hg⁰) by transition metal modified SCR catalysts was investigated by using the simulated SCR reactor. The physical and chemical properties of the catalysts were characterized by N₂ adsorption-desorption and X-ray diffraction (XRD). The results show that the specific surface area and total pore volume of the catalysts are decreased after the modification by metal oxide. However, the pore structure and distribution after modification have little variation. The weak diffraction peaks of transition metal oxide can be seen from the XRD pattern. Both 8% Ce/SCR and 8% Cu/SCR catalysts show a relatively stable and high Hg⁰ oxidation efficiency, while the oxidation activity of the 8% Co/SCR catalyst is greatly influenced by temperature. The modified SCR catalysts have an excellent catalytic performance for the Hg⁰ oxidation under a lower concentration of NH₃ and NO. And the Hg⁰ oxidation efficiency is promoted significantly in the presence of HCl. On the contrary, there is little improvement in the Hg⁰ oxidation by HCl at the condition of higher concentration of NH₃ and NO.
- metal modifier,
- SCR catalyst,
- Hg⁰ oxidation
1. [1]
  LI P, FENG X B, QIU G L, SHANG L H, LI Z G. Mercury pollution in Asia:A review of the contaminated sites[J]. J Hazrad Mater, 2009,168(2/3):591-601.
2. [2]
  SENIOR C L, HELBLE J J, SAROFIM A F. Emissions of mercury, trace elements, and fine particles from stationary combustion sources[J]. Fuel Process Technol, 2000,65-66(0):263-288.
3. [3]
  PRESTO A A, GRANITE0 E J. Survey of catalysts for oxidation of mercury in flue gas[J]. Environ Sci Technol, 2006,40(18):5601-5609. doi: 10.1021/es060504i
4. [4]
  LIU Ling, DUAN Yu-feng, WANG Yun-jun, WANG Hui, YIN Jian-jun. Experimental study on mercury release behavior and speciation during pyrolysis of two different coals[J]. J Fuel Chem Technol, 2010,38(2):134-139. doi: 10.1016/S1872-5813(10)60026-6
5. [5]
  PENG Y, SI W Z, LI X, LUO J M, LI J H, CRITTENDEN J, HAO J M. Comparison of MoO₃ and WO₃ on arsenic poisoning V₂O₅/TiO₂ catalyst:DRIFTS and DFT study[J]. Appl Catal B:Environ, 2016,181:692-698. doi: 10.1016/j.apcatb.2015.08.030
6. [6]
  PUDASAINEE D, LEE S J, LEE S H, KIM J H, JANG H N, CHO S J, SEO Y C. Effect of selective catalytic reactor on oxidation and enhanced removal of mercury in coal-fired power plants[J]. Fuel, 2010,89(4):804-809. doi: 10.1016/j.fuel.2009.06.022
7. [7]
  CAO Y, GAO Z Y, ZHU J S, WANG Q H, HUANG Y J, CHIU C C, PARKER B, CHU P, PAN W P. Impacts of halogen additions on mercury oxidation, in a slipstream selective catalyst reduction (SCR), reactor when burning sub-bituminous coal[J]. Environ Sci Technol, 2008,42(1):256-261. doi: 10.1021/es071281e
8. [8]
  CAO Y, C B, WU J, CUI H, SMITH J, CHEN C K, CH UP, PAN W P. Study of mercury oxidation by a selective catalytic reduction catalyst in a pilot-scale slipstream reactor at a utility boiler burning bituminous coal[J]. Energy Fuels, 2007,21:145-156. doi: 10.1021/ef0602426
9. [9]
  YANG H M, PAN W P. Transformation of mercury speciation through the SCR system in power plants[J]. J Environ Sci, 2007,19(2):181-184. doi: 10.1016/S1001-0742(07)60029-1
10. [10]
  SENIOR C L. Oxidation of mercury across selective catalytic reduction catalysts in coal-fired power plants[J]. J Air Waste Manage, 2006,56(1):23-31. doi: 10.1080/10473289.2006.10464437
11. [11]
  KAMATA H, UENO S I, NAITO T, YUKIMURA A. Mercury oxidation over the V₂O₅(WO₃)/TiO₂ commercial SCR catalyst[J]. Ind Eng Chem Res, 2008,47(21):8136-8141. doi: 10.1021/ie800363g
12. [12]
  YANG J, YANG Q, SUN J, LIU Q C, ZHAO D, GAO W, LIU L. Effects of mercury oxidation on V₂O₅-WO₃/TiO₂ catalyst properties in NH₃-SCR process[J]. Catal Commun, 2015,59:78-82. doi: 10.1016/j.catcom.2014.09.049
13. [13]
  LI Jian-rong, HE Chi, SHANG Xue-song, CHEN Jin-sheng, YU Xiao-wei, YAO Yuan-jun. Oxidation efficiency of elemental mercury in flue gas by SCR De-NO_x catalysts[J]. J Fuel Chem Technol, 2012,40(2):241-246. doi: 10.1016/S1872-5813(12)60012-7
14. [14]
  LI H L, LI Y, WU C Y, ZHANG J Y. Oxidation and capture of elemental mercury over SiO₂-TiO₂-V₂O₅ catalysts in simulated low-rank coal combustion flue gas[J]. Chem Eng J, 2011,169(1/3):186-193.
15. [15]
  LI H L, WU C Y, LI Y, ZHANG J Y. Superior activity of MnO_x-CeO₂/TiO₂ catalyst for catalytic oxidation of elemental mercury at low flue gas temperatures[J]. Appl Catal B:Environ, 2012,111-112:381-388. doi: 10.1016/j.apcatb.2011.10.021
16. [16]
  XU W X, WANG H R, ZHOU X, ZHU T Y. CuO/TiO₂ catalysts for gas-phase Hg⁰ catalytic oxidation[J]. Chem Eng J, 2014,243:380-385. doi: 10.1016/j.cej.2013.12.014
17. [17]
  LI H L, WU S K, WU C Y, WANG J, LI L Q, SHIH K. SCR atmosphere induced reduction of oxidized mercury over CuO/CeO₂-TiO₂ catalyst[J]. Environ Sci Technol, 2015,49(12):7373-7379. doi: 10.1021/acs.est.5b01104
18. [18]
  DRANGA B A, KOESER H. Increased co-oxidation activity for mercury under hot and cold site coal power plant conditions-Preparation and evaluation of Au/TiO₂-coated SCR-DeNO_x catalysts[J]. Appl Catal B:Environ, 2015,166-167:302-312. doi: 10.1016/j.apcatb.2014.11.018
19. [19]
  WANG P Y, SU S, XIANG J, CAO F, SUN L S, HU S, LEI S Y. Catalytic oxidation of Hg⁰ by CuO-MnO₂-Fe₂O₃/γ-Al₂O₃ catalyst[J]. Chem Eng J, 2013,225(0):68-75.
20. [20]
  WEN X Y, LI C T, FAN X P, GAO H L, ZHANG W, CHEN L, ZENG G M, ZHAO Y P. Experimental study of gaseous elemental mercury removal with CeO₂/γ-Al₂O₃[J]. Energy Fuels, 2011,25(7):2939-2944. doi: 10.1021/ef200144j
21. [21]
  XIE Y N, LI C T, ZHAO L K, ZHANG J, ZENG G M, ZHANG X N, ZHANG W, TAO S S. Experimental study on Hg⁰ removal from flue gas over columnar MnO_x-CeO₂/activated coke[J]. Appl Surf Sci, 2015,333:59-67. doi: 10.1016/j.apsusc.2015.01.234
22. [22]
  WANG J W, YANG J L, LIU Z Y. Gas-phase elemental mercury capture by a V₂O₅/AC catalyst[J]. Fuel Process Technol, 2010,91(6):676-680. doi: 10.1016/j.fuproc.2010.01.017
23. [23]
  ZHAO Li, HE Qing-song, LI Lin, LU Qiang, DONG Chang-qing, YANG Yong-ping. Research on the catalytic oxidation of Hg⁰ by modified SCR catalysts[J]. J Fuel Chem Technol, 2015,43(5):628-634. doi: 10.1016/S1872-5813(15)30018-9
24. [24]
  LIU Y, WANG Y J, WANG H Q, WU Z B. Catalytic oxidation of gas-phase mercury over Co/TiO₂ catalysts prepared by sol-gel method[J]. Catal Commun, 2011,12(14):1291-1294. doi: 10.1016/j.catcom.2011.04.017
25. [25]
  HONG H J, HAM S W, KIM M H, LEE S M, LEE J B. Characteristics of commercial selective catalytic reduction catalyst for the oxidation of gaseous elemental mercury with respect to reaction conditions[J]. Korean J Chem Eng, 2010,27(4):1117-1122. doi: 10.1007/s11814-010-0175-x
26. [26]
  LEE W, BAE G N. Removal of elemental mercury (Hg (0)) by nanosized V₂O₅/TiO₂ catalysts[J]. Environ Sci Technol, 2009,43(5):1522-1527. doi: 10.1021/es802456y
27. [27]
  GAO X, JIANG Y, ZHONG Y, LUO Z Y, CEN K F. The activity and characterization of CeO₂-TiO₂ catalysts prepared by the sol-gel method for selective catalytic reduction of NO with NH₃[J]. J Hazrad Mater, 2010,174:734-739. doi: 10.1016/j.jhazmat.2009.09.112
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1.
沈阳化工大学材料科学与工程学院沈阳 110142