Skip to main content
Log in

Heterogeneous oxidation of carbonyl sulfide on mineral oxides

  • Articles
  • Environmental Chemistry
  • Published:
Chinese Science Bulletin

Abstract

Heterogeneous oxidation of carbonyl sulfide (OCS) on mineral oxides including SiO2, Fe2O3, CaO, MgO, ZnO and TiO2, which are the main components of atmospheric particles, were investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), ion chromatography (IC), temperature-programmed desorption (TPD), X-ray diffraction (XRD) and Brunauer-Emmett-Teller (BET) methods. The main products and intermediates of the heterogeneous oxidation of OCS on these oxides were identified with in situ DRIFTS and IC. The reaction mechanism and kinetics were also discussed. It is found that the reaction mechanism on these mineral oxides is the same as that on Al2O3 for the same final products and the intermediates at room temperature. Namely, OCS can be catalytically oxidized to produce surface SO 2−4 species and gaseous CO2 through the surface hydrogen thiocarbonate (HSCO 2 ) and HSO 3 species. The activity series for heterogeneous oxidation of OCS follows: Al2O3 ≈ CaO > MgO > TiO2 ≈ ZnO > Fe2O3 > SiO2. The specific area, basic hydroxyl and surface basicity of these oxides have effect on the reactivity. This study suggests that heterogeneous reactions of OCS on mineral dust may be an unneglectable sink of OCS.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Similar content being viewed by others

References

  1. Turco R P, Whitten R C, Toon O B, et al. Stratospheric aerosols and climate. Nature, 1980, 283: 283–285

    Article  Google Scholar 

  2. Andreae M O, Crutzen P J. Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry. Science, 1997, 276: 1052–1058

    Article  Google Scholar 

  3. Crutzen P J. The possible importance of CSO for the sulfate layer of the stratosphere. Geophys Res Lett, 1976, 3: 73–76

    Google Scholar 

  4. Watts S F. The mass budgets of carbonyl sulfide, dimethyl sulfide, carbon disulfide and hydrogen sulfide. Atmos Environ, 2000, 34(5): 761–779

    Article  Google Scholar 

  5. Yang W X, Mu Y J, Liu Y, et al. Ozone depletion rate on ice surface at low temperature. Chin Sci Bull, 1996, 41(4): 343–345

    Google Scholar 

  6. Mu Y J, Liu Y, Yang W X. The stickin coefficients of ozone onice and doped ice. Acta Sci Cirtumstan (in Chinese), 2000, 20(4): 410–414

    Google Scholar 

  7. Ravishankara A R. Heterogeneous and multiphase chemistry in the troposphere. Science, 1997, 276: 1058–1064

    Article  Google Scholar 

  8. Ding J, Zhu T. Heterogeneous reactions on the surface of fine particles in atmosphere. Chin Sci Bull, 2003, 48(21): 2267–2276

    Article  Google Scholar 

  9. Wang L, Zhang F, Cheng J M. Heterogeneous catalysis reaction between carbon disulfide and atmospheric particles. Chem J Chin Univ (in Chinese), 2002, 23(5): 866–870

    Google Scholar 

  10. Lin G Z, Mao S S, Wang Q G Powder X-ray diffraction analysis of atmospheric particles in Beijing. Acta Sci Circumstan (in Chinese), 1983, 3(4): 311–318

    Google Scholar 

  11. Zhang Z, Friedlander S K. A comparative study of chemical databases for fine particle Chinese aerosols. Environ Sci Technol, 2000, 34(22): 4687–4694

    Article  Google Scholar 

  12. Gordon E B J. How minerals react with water. Science, 2001, 294: 67–70

    Article  Google Scholar 

  13. Tang X Y. Atmospheric Envrionmental Chemistry (in Chinese). Beijing: Higher Education Press, 1990. 182

    Google Scholar 

  14. Wu H B, Wang X, Cheng J M, et al. Mechanism of the heterogeneous reaction of carbonyl sulfide with typical components of atmospheric aerosol. Chin Sci Bull, 2004, 49(12): 1231–1235

    Article  Google Scholar 

  15. He H, Liu J F, Mu Y J, et al. Heterogeneous oxidation of carbonyl sulfide on atmospheric particles and alumina. Environ Sci Technol, 2005, 39(24): 9637–9642

    Article  Google Scholar 

  16. Peri J B, Hannan R B. Surface hydroxyl groups on γ-alumina. J Phys Chem, 1960, 64(10): 1526–1530

    Article  Google Scholar 

  17. Ballinger T H, Yates J J T. IR spectroscopic detection of Lewis acid sites on alumina using adsorbed carbon monoxide: Correlation with aluminum-hydroxyl group removal. Langmuir, 1991, 7(12): 3041–3045

    Article  Google Scholar 

  18. Lavalley J C, Travert J, Chevreau T, et al. Infrared study of coadsorption of H2S and CO2 on γ-alumina. J Chem Soc Chem Comm, 1979, (4): 146–148

  19. Hoggan P E, Aboulayt A, Pieplu A, et al. Mechanism of COS hydrolysis on alumina. J Catal, 1994, 149(2): 300–306

    Article  Google Scholar 

  20. Saur O, Bensitel M, Mohammed Saad A B, et al. The structure and stability of sulfated alumina and titania. J Catal, 1986, 99(1): 104–110

    Article  Google Scholar 

  21. Lavalley J C. Infrared spectrometric studies of the surface basicity of metal oxides and zeolites using adsorbed probe molecules. Catal Today, 1996, 27(3–4): 377–401

    Article  Google Scholar 

  22. Goodman A L, Li P, Usher C R, et al. Heterogeneous uptake of sulfur dioxide on aluminum and magnesium oxide particles. J Phys Chem A, 2001, 105(25): 6109–6120

    Article  Google Scholar 

  23. Amenomiya Y, Morikawa Y, Pleizier G Infrared spectroscopy of C18O2 on alumina. J Catal, 1977, 46(3): 431–433

    Article  Google Scholar 

  24. Rege S U, Yang R T. A novel FTIR method for studying mixed gas adsorption at low concentrations: H2O and CO2 on NaX zeolite and γ-alumina. Chem Eng Sci, 2001, 56(12): 3781–3796

    Article  Google Scholar 

  25. Chang C C. Infrared studies of SO2 on γ-alumina. J Catal, 1978, 53(3): 374–385

    Article  Google Scholar 

  26. Turek A M, Wachs I E, DeCanio E. Acidic properties of alumina-supported metal oxide catalysts: An infrared spectroscopy study. J Phys Chem, 1992, 96(12): 5000–5007

    Article  Google Scholar 

  27. Liu J F, Yu Y B, Mu Y J, et al. Mechanism of heterogeneous oxidation of carbonyl sulfide on Al2O3: An in situ diffuse reflectance infrared Fourier transform spectroscopy investigation. J Phys Chem B, 2006, 110: 3225–3230

    Article  Google Scholar 

  28. Wu Y. Catalysis Chemistry (in Chinese). Vol. 1. Beijing: Science Press, 2000. 188

    Google Scholar 

Download references

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to He Hong.

Additional information

Supported by the Ministry of Science and Technology of China (Grant No. 2007CB 407301) and the National Natural Science Foundation of China (Grant No. 20637001)

About this article

Cite this article

Liu, Y., Liu, J., He, H. et al. Heterogeneous oxidation of carbonyl sulfide on mineral oxides. CHINESE SCI BULL 52, 2063–2071 (2007). https://doi.org/10.1007/s11434-007-0281-2

Download citation

  • Received:

  • Accepted:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11434-007-0281-2

Keywords

Navigation