Advertisement

Reaction Kinetics, Mechanisms and Catalysis

, Volume 124, Issue 2, pp 669–682 | Cite as

Selective catalytic reduction of SO2 with methane for recovery of elemental sulfur over nickel-alumina catalysts

  • Seyyed Ebrahim Mousavi
  • Hassan Pahlavanzadeh
  • Masoud Khani
  • Habib Ale Ebrahim
  • Abbas Mozaffari
Article

Abstract

In the current research, to form elemental sulfur, catalytic reduction of sulfur dioxide with methane over Ni–Al2O3 catalysts was studied. By adding nickel as a promoter, the performance of catalyst was enhanced considerably. It was found that Al2O3–Ni (10%) catalyst had the best performance among all the catalysts studied. The addition of more than 10% Ni had no beneficial effect. The reaction was tested at temperature range of 550–800 °C, at the atmospheric pressure, and it was observed that complete conversion and selectivity (more than 99.5%) was achieved by Al2O3–Ni(10%) catalyst at 750 °C. Between molar feed ratio of SO2/CH4 = 1–3, the highest conversion to elemental sulfur combined with low production of H2S and COS, as the undesirable side products, was obtained when molar ratio was equal to 2 (the stoichiometric ratio). Also, the best catalyst showed good long-term stability for SO2 reduction with methane.

Keywords

Sulfur dioxide removal Nickel-alumina catalyst SO2 Reduction by CH4 Elemental sulfur recovery Catalyst reduction Nickel nanoparticles on alumina 

References

  1. 1.
    Davis D, Kemp D (1991) Kirk-othmer encyclopedia of chemical technology. Wiley, New YorkGoogle Scholar
  2. 2.
    Wang G, Bing L, Yang Z, Zhang J (2014) Selective catalytic reduction of sulfur dioxide by carbon monoxide over iron oxide supported on activated carbon. Turk J Chem 38(1):70–78CrossRefGoogle Scholar
  3. 3.
    Zhao H, Luo X, He J, Peng C, Wu T (2015) Recovery of elemental sulphur via selective catalytic reduction of SO2 over sulphided CoMo/γ-Al2 O3 catalysts. Fuel 147:67–75CrossRefGoogle Scholar
  4. 4.
    Chen C-L, Wang C-H, Weng H-S (2004) Supported transition-metal oxide catalysts for reduction of sulfur dioxide with hydrogen to elemental sulfur. Chemosphere 56(5):425–431CrossRefGoogle Scholar
  5. 5.
    Han GB, Park N-K, Yoon SH, Lee TJ, Han GY (2008) Direct reduction of sulfur dioxide to elemental sulfur with hydrogen over Sn–Zr-based catalysts. Ind Eng Chem Res 47(14):4658–4664CrossRefGoogle Scholar
  6. 6.
    Jin Y, Yu Q, Chang SG (1997) Reduction of sulfur dioxide by syngas to elemental sulfur over iron-based mixed oxide supported catalyst. Environ Prog 16(1):1–8CrossRefGoogle Scholar
  7. 7.
    Helstrom JJ, Atwood GA (1978) The kinetics of the reaction of sulfur dioxide with methane over a bauxite catalyst. Ind Eng Chem Process Des Dev 17(2):114–117CrossRefGoogle Scholar
  8. 8.
    Bobrin A, Anikeev V, Yermakova A, Kirillov V (1989) High-temperature reduction of SO2 by methane at various CH4/SO2 ratios. React Kinet Catal Lett 40(2):363–367CrossRefGoogle Scholar
  9. 9.
    Sarlis J, Berk D (1988) Reduction of sulfur dioxide with methane over activated alumina. Ind Eng Chem Res 27(10):1951–1954CrossRefGoogle Scholar
  10. 10.
    Bobrin A, Anikeev V, Yermakova A, Zheivot V, Kirillov V (1989) Kinetic studies of high-temperature reduction of sulfur dioxide by methane. React Kinet Catal Lett 40(2):357–362CrossRefGoogle Scholar
  11. 11.
    Mulligan DJ, Berk D (1992) Reduction of sulfur dioxide over alumina-supported molybdenum sulfide catalysts. Ind Eng Chem Res 31(1):119–125CrossRefGoogle Scholar
  12. 12.
    Mulligan DJ, Tam K, Berk D (1995) A study of supported molybdenum catalysts for the reduction of SO2 with CH4: effect of sulphidation method. Can J Chem Eng 73(3):351–356CrossRefGoogle Scholar
  13. 13.
    Wiltowski TS, Sangster K, O’Brien WS (1996) Catalytic reduction of SO2 with methane over molybdenum catalyst. J Chem Technol Biotechnol 67(2):204–212CrossRefGoogle Scholar
  14. 14.
    Sarlis J, Berk D (1995) Reduction of sulphur dioxide by methane over transition metal oxide catalysts. Chem Eng Commun 140(1):73–85CrossRefGoogle Scholar
  15. 15.
    Zhang X, Hayward DO, Lee C, Mingos DMP (2001) Microwave assisted catalytic reduction of sulfur dioxide with methane over MoS 2 catalysts. Appl Catal B 33(2):137–148CrossRefGoogle Scholar
  16. 16.
    Zhu T, Dreher A, Flytzani-Stephanopoulos M (1999) Direct reduction of SO 2 to elemental sulfur by methane over ceria-based catalysts. Appl Catal B 21(2):103–120CrossRefGoogle Scholar
  17. 17.
    Zhu T, Kundakovic L, Dreher A, Flytzani-Stephanopoulos M (1999) Redox chemistry over CeO 2-based catalysts: SO 2 reduction by CO or CH 4. Catal Today 50(2):381–397CrossRefGoogle Scholar
  18. 18.
    Flytzani-Stephanopoulos M, Zhu T, Li Y (2000) Ceria-based catalysts for the recovery of elemental sulfur from SO 2-laden gas streams. Catal Today 62(2):145–158CrossRefGoogle Scholar
  19. 19.
    Mousavi S, Ebrahim HA, Edrissi M (2014) Preparation of high surface area Ce/La/Cu and Ce/La/Ni ternary metal oxides as catalysts for the SO2 reduction by CH4. Synth React Inorg Met-Org Nano-Met Chem 44(6):881–890CrossRefGoogle Scholar
  20. 20.
    Mulligan DJ, Berk D (1989) Reduction of sulfur dioxide with methane over selected transition metal sulfides. Ind Eng Chem Res 28(7):926–931CrossRefGoogle Scholar
  21. 21.
    Shikina N, Khairulin S, Yashnik S, Teryaeva T, Ismagilov Z (2015) Direct catalytic reduction of SO2 by CH4 over Fe-Mn catalysts prepared by granulation of ferromanganese nodules. Eurasian Chem Technol J 17(2):129–136CrossRefGoogle Scholar
  22. 22.
    Yu J-J, Yu Q, Jin Y, Chang S-G (1997) Reduction of sulfur dioxide by methane to elemental sulfur over supported cobalt catalysts. Ind Eng Chem Res 36(6):2128–2133CrossRefGoogle Scholar
  23. 23.
    Becerra AM, Iriarte ME, Luna AEC (2003) Catalytic activity of a nickel on alumina catalyst in the CO2 reforming of methane. React Kinet Catal Lett 79(1):119–125CrossRefGoogle Scholar
  24. 24.
    Yenumala SR, Maity SK, Shee D (2017) Reaction mechanism and kinetic modeling for the hydrodeoxygenation of triglycerides over alumina supported nickel catalyst. Reac Kinet Mech Cat 120(1):109–128CrossRefGoogle Scholar
  25. 25.
    Ebrahim HA, Jamshidi E (2004) Synthesis gas production by zinc oxide reaction with methane: elimination of greenhouse gas emission from a metallurgical plant. Energy Convers Manag 45(3):345–363CrossRefGoogle Scholar
  26. 26.
    Hernández Guiance SN, Coria ID, Irurzun IM, Mola EE (2016) Experimental determination of the activation energies of CH4, SO2 and O2 reactions on Cr2O3/γ -Al2O3. Chem Phys Lett 660:123–126CrossRefGoogle Scholar

Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2018

Authors and Affiliations

  • Seyyed Ebrahim Mousavi
    • 1
  • Hassan Pahlavanzadeh
    • 1
  • Masoud Khani
    • 2
  • Habib Ale Ebrahim
    • 2
  • Abbas Mozaffari
    • 3
  1. 1.Faculty of Chemical EngineeringTarbiat Modares UniversityTehranIran
  2. 2.Faculty of Chemical Engineering, Petrochemical Center of ExcellencyAmirkabir University of TechnologyTehranIran
  3. 3.Research and Development UnitSarcheshmeh Copper ComplexKermanIran

Personalised recommendations