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Environmental Science and Pollution Research

, Volume 26, Issue 10, pp 9686–9696 | Cite as

Study of MoO3-γAl2O3 catalysts behavior in selective catalytic reduction of SO2 toxic gas to sulfur with CH4

  • Masoud Khani
  • Seyyed Ebrahim MousaviEmail author
  • Hassan PahlavanzadehEmail author
  • Habib Ale Ebrahim
  • Abbas Mozaffari
Research Article
  • 76 Downloads

Abstract

In the present study, a detailed investigation was carried out on MoO3 alumina-supported catalysts behavior in selective catalytic reduction of SO2 to sulfur with CH4. At first, four different molybdenum catalysts with weight rates of 0, 5, 10, and 15 were impregnated on γ-alumina to be characterized using XRD, SEM, BET, BJH, and N2 adsorption. Then, to find the most active catalyst, temperature dependency test was performed on all of the prepared catalysts and the result representing Al2O3-Mo10 as the best catalyst. In next step, the effects of feed gas composition, space velocity, and long-term activity, as an important industrial factor, were tested on Al2O3-Mo10. It was revealed instantaneously from the beginning, MoO3 specie started to convert mainly into MoS2 and MoO2, and a minor part into Mo2C, which is terminated after 750 min achieving a stable condition. Thereafter, SO2 conversion and sulfur selectivity increased from 85.8 to 89.4% and 99.4 to 99.7%, respectively. XRD graph of the used catalyst and TPO thermogravimetric/mass-spectra proved possible happening of the proposed mechanism in long-term activity. At the end, mean activation energy was determined based on Arrhenius model in temperature range of 550 to 800 °C, with a value of 0.33 eV for Al2O3-Mo10.

Keywords

Molybdenum-alumina catalyst Catalytic reduction of SO2 Sulfur dioxide removal SO2 reduction by CH4 Elemental sulfur recovery Molybdenum oxide nanoparticles on alumina 

Notes

References

  1. Ahmad H, Ismail MA, Suthaskumar M, Tiu ZC, Harun SW, Zulkifli MZ, Samikannu S, Sivaraj S (2016) S-band Q-switched fiber laser using molybdenum disulfide (MoS2) saturable absorber. Laser Phys Lett 13:1–7Google Scholar
  2. Ale Ebrahim H, Jamshidi E (2004) Synthesis gas production by zinc oxide reaction with methane: elimination of greenhouse gas emission from a metallurgical plant. Energy Convers Manag 45:345–363CrossRefGoogle Scholar
  3. Alemán-Vázqueza LO, Torres-García E, Villagómez-Ibarra JR, Cano-Domínguez JL (2005) Effect of the particle size on the activity of MoOxCy catalysts for the isomerization of heptane. Catal Lett 100:219–224CrossRefGoogle Scholar
  4. Chen CL, Wang CH, Weng HS (2004) Supported transition-metal oxide catalysts for reduction of sulfur dioxide with hydrogen to elemental sulfur. Chemosphere 56:425–431CrossRefGoogle Scholar
  5. Chen C, Yoza BA, Wang Y, Wang P, Li QX, Guo S, Yan G (2015) Catalytic ozonation of petroleum refinery wastewater utilizing Mn-Fe-Cu/Al2O3 catalyst. Environ Sci Pollut Res 22:5552–5562CrossRefGoogle Scholar
  6. Dowling NI, Hyne JB, Brown DM (1990) Kinetics of the reaction between hydrogen and sulfur under high-temperature Claus furnace conditions. Ind Eng Chem Res 29:2327–2332CrossRefGoogle Scholar
  7. Du J, Wu J, Guo T, Zhao R, Li J (2014) Catalytic performance of Mo2C supported on onion-like carbon for dehydrogenation of cyclohexane. RSC Adv 4:53950–53953CrossRefGoogle Scholar
  8. Feng T, Zhao X, Wang T, Xia X, Zhang M, Huan Q, Ma C (2016) Reduction of SO2 with CO to elemental sulfur in activated carbon bed. Energy Fuel 30:6578–6584CrossRefGoogle Scholar
  9. Feng T, Huo M, Zhao X, Wang T, Xia X, Ma C (2017) Reduction of SO2 to elemental sulfur with H2 and mixed H2/CO gas in an activated carbon bed. Chem Eng Res Des 121:191–199CrossRefGoogle Scholar
  10. Flytzani-Stephanopoulos M, Zhu T, Li Y (2000) Ceria-based catalysts for the recovery of elemental sulfur from SO2-laden gas streams. Catal Today 62:145–158CrossRefGoogle Scholar
  11. Gao G, Wei S, Duan X, Pan X (2015) Influence of charge state on catalytic properties of PtAu(CO)n in reduction of SO2 by CO. Chem Phys Lett 625:128–131CrossRefGoogle Scholar
  12. Ge T, Zuo C, Zhang J, Wei L, Li C (2018) Selective reduction of SO2 in smelter off-gas with coal gas to sulfur over metal sulfide supported catalysts. Ind Eng Chem Res 57:4170–4179CrossRefGoogle Scholar
  13. Guiance SH, 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
  14. Guldal NO, Figen HE, Baykara SZ (2017) Production of hydrogen from hydrogen sulfide with perovskite type catalysts: LaMO3. Chem Eng J 313:1354–1363CrossRefGoogle Scholar
  15. Hibbert DB, Campbell RH (1988) Flue gas desulphurisation: catalytic removal of sulphur dioxide by carbon monoxide on sulphided La1−xSrxCoO3: II. Reaction of sulphur dioxide and carbon monoxide in a flow system. Appl Catal 41:289–299CrossRefGoogle Scholar
  16. Homsi D, Abou Rached J, Aouad S, Gennequin C, Dahdah E, Estephane J, Lucette Tidahy H, Aboukaïs A, Abi-Aad E (2017) Steam reforming of ethanol for hydrogen production over Cu/Co-Mg-Al-based catalysts prepared by hydrotalcite route. Environ Sci Pollut Res 24:9907–9913CrossRefGoogle Scholar
  17. Lam FLY, Fu MO, Hu X (2010) Superior adsorption capacity of film typed carbon for the abatement of sulfur dioxide. Catal Today 158:269–272CrossRefGoogle Scholar
  18. Liu Y, Bisson TM, Yang H, Xu Z (2010) Recent developments in novel sorbents for flue gas clean up. Fuel Process Technol 91:1175–1197CrossRefGoogle Scholar
  19. Mousavi SE, Ale Ebrahim H, 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-Metal Chem 44:881–890CrossRefGoogle Scholar
  20. Mousavi SE, Pahlavanzadeh H, Ale Ebrahim H (2017) Preparation, characterization and optimization of high surface area Ce-La-Cu ternary oxide nanoparticles. E-J Surf Sci Nanotechnol 15:87–92CrossRefGoogle Scholar
  21. Mousavi SE, Pahlavanzadeh H, Khani M, Ale Ebrahim H, Mozaffari A (2018) Selective catalytic reduction of SO2 with methane for recovery of elemental sulfur over nickel-alumina catalysts. React Kinet Mech Catal 124:1–14CrossRefGoogle Scholar
  22. Mulligan DJ, Berk D (1992) Reduction of sulfur dioxide over alumina-supported molybdenum sulfide catalysts. Ind Eng Chem Res 31:119–125CrossRefGoogle Scholar
  23. 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 73:351–356CrossRefGoogle Scholar
  24. Paik SC, Chung JS (1995) Selective catalytic reduction of sulfur dioxide with hydrogen to elemental sulfur over Co-Mo/Al2O3. Appl Catal B Environ 5:233–243CrossRefGoogle Scholar
  25. Sarlis J, Berk D (1988) Reduction of sulfur dioxide with methane over activated alumina. Ind Eng Chem Res 27:1951–1954CrossRefGoogle Scholar
  26. Sarlis J, Berk D (1995) Reduction of sulphur dioxide by methane over transition metal oxide catalysts. Chem Eng Commun 140:73–85CrossRefGoogle Scholar
  27. 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 17:129–136CrossRefGoogle Scholar
  28. Sundeep D, Gopala Krishna A, Ravikumar RVSSN, Vijaya Kumar T, Daniel Ephraim S, Pavan YL (2016) Spectral characterization of mechanically synthesized MoO3-CuO nanocomposite. Int Nano Lett 6:119–128CrossRefGoogle Scholar
  29. Tailor R, Sayari A (2016) Grafted propyldiethanolamine for selective removal of SO2 in the presence of CO2. Chem Eng J 289:142–149CrossRefGoogle Scholar
  30. Voitovich R, Pugach E (1973) High-temperature oxidation characteristics of the carbides of the group VI transition metals. Powder Metall Met Ceram 12:314–318CrossRefGoogle Scholar
  31. Wang CH, Lin SS, Sung PC, Weng HS (2003) Catalytic reduction of SO2 over supported transition-metal oxide catalysts with C2H4 as a reducing agent. Appl Catal B Environ 40:331–345CrossRefGoogle Scholar
  32. Yermakova A, Anikeev V, Bobrin A (1993) Kinetic model for the reaction of sulphur dioxide catalytic reduction to hydrogen sulphide. Appl Catal A Gen 101:25–39CrossRefGoogle Scholar
  33. Yu JJ, Yu Q, Jin Y, Chang SG (1997) Reduction of sulfur dioxide by methane to elemental sulfur over supported cobalt catalysts. Ind Eng Chem Res 36:2128–2133CrossRefGoogle Scholar
  34. 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-Al2O3 catalysts. Fuel 147:67–75CrossRefGoogle Scholar
  35. Zhu T, Dreher A, Flytzani-Stephanopoulos M (1999) Direct reduction of SO2 to elemental sulfur by methane over ceria-based catalysts. Appl Catal B Environ 21:103–120CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

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

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