Start Submission Become a Reviewer

Reading: Sulfur (32S, 33S, 34S, 36S) and oxygen (16O, 17O, 18O) isotopic ratios of primary sulfate pr...

Download

A- A+
Alt. Display

Original Research Papers

Sulfur (32S, 33S, 34S, 36S) and oxygen (16O, 17O, 18O) isotopic ratios of primary sulfate produced from combustion processes

Authors:

C. C.-W. Lee ,

Department of Chemistry and Biochemistry, University of California — San Diego, US
X close

J. Savarino,

Department of Chemistry and Biochemistry, University of California — San Diego, US; L aboratoire de Glaciologie et Géophysique de l’Environnement, FR
X close

H. Cachier,

L aboratoire des Sciences du Climat et de l’Environnement, FR
X close

M. H. Thiemens

Department of Chemistry and Biochemistry, University of California — San Diego, US
X close

Abstract

The recent discovery of an anomalous enrichment in 17O isotope in atmospheric sulfate has opened a new way to investigate the oxidation pathways of sulfur in the atmosphere. From laboratory investigations, it has been suggested that the wet oxidation of sulfur in rain droplets was responsible for the excess 17O. In order to confirm this theory, sulfur and oxygen isotope ratios of different primary sulfates produced during fossil fuel combustion have been investigated and are reported. None of these samples exhibits any anomalous oxygen or sulfur isotopic content, as compared to urban sulfate aerosols. These results, in agreement with the laboratory investigations, reinforce the idea of an aqueous origin for the oxygen-17 anomaly found in tropospheric sulfates.

How to Cite: Lee, C.C.-W., Savarino, J., Cachier, H. and Thiemens, M.H., 2002. Sulfur (32S, 33S, 34S, 36S) and oxygen (16O, 17O, 18O) isotopic ratios of primary sulfate produced from combustion processes. Tellus B: Chemical and Physical Meteorology, 54(3), pp.193–200. DOI: http://doi.org/10.3402/tellusb.v54i3.16660
2
Views
1
Downloads
  Published on 01 Jan 2002
 Accepted on 28 Jan 2002            Submitted on 4 Oct 2001

References

  1. Bains-Sahota , S. K. and Thiemens , M. H . 1989 . A mass-independent sulfur isotope effect in the nonthermal formation of sulfur fluoride (S2 F10). J. Chem. Phys . 90 , 6099 – 6109 .  

  2. Bhattacharya , S. K. and Thiemens , M. H . 1989 . New evidence for symmetry dependent isotope effect: 0 + CO Reaction. Z. Naturforcsh., Teil A 44A , 435 – 444 .  

  3. Burdett , N. A. , Gliddon , B. J. , Hotchkiss , R. C. and Squires , R. T . 1983 . Sulfur trioxide in coal-fired fluidized-bed combustors. J. Inst. Energy 56 , 119 – 124 .  

  4. Calhoun , J. A. , Bates , T. S. and Charlson , R. J . 1991 . Sulfur isotope measurements of submicrometer sulfate aerosol particles over the Pacific ocean. Geophys. Res. Lett . 18 , 1877 – 1880 .  

  5. Chuang , C. C. , Penner , J. E. , Taylor , K. E. , Grossman , A. S. and Walton , J. J . 1997 . An assessment of the radiative effects of anthropogenic sulfate. J. Geophys. Res . 102 , D3 , 3761 – 3778 .  

  6. Colman , J. J. , Xu , X. P. , Thiemens , M. H. and Trogler , W. C . 1996 . Photopolymerization and mass-independ-ent sulfur isotope fractionations in carbon disulfide. Science 273 , 774 – 776 .  

  7. Cullis , C. F. and Mulcahy , M. F. R . 1972 . Kinetics of combustion of gaseous sulfur compounds. Combust. Flame 18 , 225 – 292 .  

  8. Farquhar , J. , Savarino , J. , Airieau , S. and Thiemens , M. H . 2002 . Observation of wavwlength-sensitive mass-independent sulfur isotope effects during SO2 photolysis: application to the early atmosphere. J. Geo-phys. Res ., 106 E12 , 32829 – 32840 .  

  9. Feichter , J. , Kjellstrom , E. , Rodhe , H. , Dentener , F. , Lelieveld , J. and Roelofs , G. J . 1996 . Simulation of the tropospheric sulfur cycle in a global climate model. Atmos. Environ . 30 , 1693 – 1707 .  

  10. Flagan , R. C. and Friedlander , S. K . 1978 . Particle forma-tion in pulverized coal combustion - a review. In: Recent developments in aerosol science (ed. D. T. Shaw). Wiley & Sons , New York , 25 – 59 .  

  11. Gao , X. and Thiemens , M. H . 1991 . Systematic study of sulfur isotopic composition in iron meteorites and the occurence of excess “S and “S. Geochim. Cosmochim. Acta 55 , 2671 – 2679 .  

  12. Hewitt , C. N . 2001 . The atmospheric chemistry of sul-phur and nitrogen in power station plumes. Atmos. Environ . 35 , 1155 – 1170 .  

  13. Holt , B. D. and Kumar , R . 1984 . Oxygen-18 study of high-temperature air oxidation of SO2. Atmos. Environ . 18 , 2089 – 2094 .  

  14. Holt , B. D. , Kumar , R. and Cunningham , P. T. 1982 . Primary sulfates in atmospheric sulfates: estimation by oxygen isotope ratio measurements. Science 217 , 51 - 53 .  

  15. Hulden , B. and Astrom , L . 1973 . Sulfate formation in magnesium sulfite-spent liquor fired boilers. Tappi 56 , 84 – 86 .  

  16. Hulston , J. R. and Thode , H. G . 1965 . Variations in the 335, 345, and 36S contents of meteorites and their rela-tions to chemical and nuclear effects. J. Geophys. Res . 70 , 3475 – 3484 .  

  17. Hunter , S. C . 1982 . Formation of sulfur trioxide in gas turbines. J. Eng. Power 104 , 44 – 51 .  

  18. Kasibhatla , P. , Chameides , W. L. and St. John , J . 1997 . A three-dimensional global model investigation of sea-sonal variations in the atmospheric burden of anthro-pogenic sulfate aerosols. J. Geophys. Res . 102 , D3 , 3737 – 3759 .  

  19. Kiehl , J. T. , Schneider , T. L. , Rasch , P. J. , Barth , M. C. and Wong , J . 2000 . Radiative forcing due to sulfate aerosols from simulations with the National Center for Atmospheric Research Community Climate Model, Version 3. J. Geophys. Res . 105 , D1 , 1441 - 1457 .  

  20. Koch , D. , Jacob , D. , Tegen , I. , Rind , D. and Mian , C . 1999 . Tropospheric sulfur simulation and sulfate direct radiative forcing in the Goddard Institute for Space Studies general circulation model. J. Geophys. Res . 104 , D19, 23,799 - 23,822 .  

  21. Krause , H. H. , Levy , A. and Reid , W. T. 1969 . Radioact-ive sulfur oxide studies of external corrosion reactions on surfaces. J. Eng. Power 91 , 216 - 222 .  

  22. Lee , C. C.-W. and Thiemens , M. H . 2001 . 5'70 and 6180 measurement of atmospheric sulfate from a coastal and high alpine region: a mass independent isotopic anomaly. J. Geophys. Res. 106 , D15, 17,359 - 17,374 .  

  23. Lee , C. C.-W. , Savarino , J. and Thiemens , M. H . 2001 . Mass independent isotopic composition of atmo-spheric sulfate: origin and implications for the present and past atmosphere of Earth and Mars. Geophys. Res. Lett . 28 , 1783 – 1786 .  

  24. Lelieveld , J. , Roelofs , G. J. , Ganzeveld , L. , Feichter , J. and Rodhe , H . 1997 . Terrestrial sources and distribu-tion of atmospheric sulfur. Philos. Trans. R. Soc. London, Ser. B 352 , 149 – 158 .  

  25. Lovejoy , E. R. , Hanson , D. R. and Huey , L. G. 1996 . Kinetics and products of the gas-phase reaction of SO3 with water. J. Phys. Chem . 100 , 19,911 - 19,916 .  

  26. Mizutani , Y . 1971 . An improvement in the carbon-reduction method for the oxygen isotopic analysis of sulphates. Geochem. J . 5 , 69 – 77 .  

  27. Newman , L. , Krouse , H. R. and Grinenko , V. A . 1991 . Sulphur isotope variation in the atmosphere, in stable isotopes: natural and anthropogenic sulphur in the envi- ronment (eds. H. R. Krouse and V. A. Grinenko). John Wiley & Sons , New York , 131 – 176 .  

  28. Ohmoto , H. , Yamaguchi , K. E. , Ono , S. , Farquhar , J. , Bao , H. , Thiemens , M. H. , Hu , G. and Rumble III, D. 2001 . Questions regarding precambrian sulfur isotope fractionation. Science 292 , 1959.  

  29. Pan , W. , Tatang , M. A. , McRae , G. J. and Prinn , R. G . 1998 . Uncertainty analysis of indirect radiative forcing by anthropogenic sulfate aerosols. J. Geophys. Res . 103 , D4 , 3815 – 3823 .  

  30. Patris , N. , Mihalopoulos , N. , Baboukas , E. D. and Jouzel , J . 2000 . Isotopic composition of sulfur in size-resolved marine aerosols above the Atlantic Ocean. J. Geophys. Res . 105 , D11 , 14,449 - 14,457 .  

  31. Rafter , T. A . 1957a . Sulphur isotopic variations in nature. Part 1 — the preparation of sulphur dioxide for mass spectrometer examination. N. Z. J. Sci. Technol. B 38 , 849 – 857 .  

  32. Rafter , T. A . 1957b . Sulphur isotopic variations in nature. Part 2 — a quantitaive study of the reduction of barium sulphate by graphite for recovery of sulphide-sulphur for sulphur isotopic measurement. N. Z. J. Sci. Technol. B 38 , 955 – 968 .  

  33. Rasch , P. J. , Barth , M. C. , Kiehl , J. T. , Schwartz , S. E. and Benkovitz , C. M . 2000 . A description of the global sulfur cycle and its controlling processes in the National Center for Atmospheric Research Commu-ity Climate Model, Version 3. J. Geophys. Res . 105 , D1 , 1367 - 1385 .  

  34. Rodhe , H . 1999 . Human impact on the atmospheric sulfur balance. Tellus 51B , 110 – 122 .  

  35. Ruellan , S. and Cachier , H . 2000 . Characterisation of fresh particulate vehicular exhausts near a Paris high flow road. Atmos. Environ . 35 , 453 – 468 .  

  36. Saltzman , E. S. , Brass , G. W. and Price , D. A . 1983 . The mechanism of sulfate aerosol formation: chemical and sulfur isotopic evidence. Geophys. Res. Lett . 10 , 513 – 516 .  

  37. Savarino , J. , Lee , C. C.-W. and Thiemens , M. H . 2000 . Laboratory oxygen isotopic study of sulfur (IV) oxida-tion: origin of the mass independent oxygen isotopic anomaly in atmospheric sulfates and other sulfate min-eral deposits. J. Geophys. Res . 15 , D23, 29,079 - 29,089 .  

  38. Seinfeld , J. H. and Pandis , S. N . 1998 . Atmospheric chem-istry and physics. John Wiley & Sons , New York , 1326 pp .  

  39. Squires , R. T . 1982 . The kinetics of sulfur trioxide formation in oil-fired boilers. J. Inst. Energy 55 , 41 - 46 .  

  40. Tanaka , N. , Rye , D. M. , Xiao , Y. and Lasaga , A. C. 1994 . Use of stable sulfur isotope systematics for evaluating oxidation reaction pathways and in-cloud scavenging of sulfur dioxide in the atmosphere. Geophys. Res. Lett . 21 , 1519 – 1522 .  

  41. Thiemens , M. H . 1999 . Mass-independent isotope effects in planetary atmospheres and the solar system. Science 283 , 341 – 345 .  

  42. Thode , H. G . 1991 . Sulphur isotopes in nature and the environment: an overview. In: Stable isotopes: natural and anthropogenic sulphur in the environment (eds. H. R. Krouse and V. A. Grimenko). John Wiley & Sons , New York , 1 – 21 .  

  43. Tschinkel , J. G . 1972 . Formation of sodium sulfate in gas turbine combustors. Corrosion 28 , 161 – 169 .  

  44. Van Dinh , P. , Serpolay , R. and Lacaux , J. P . 1996 . Labor-atory investigations on aerosols from the combustion of savanna grass and cereal straw. In: Biomass burning and global change (ed. J. L. Levine). MIT Press, Cambridge, MA, 472 - 484 .  

  45. van Dorland , R. , Dentener , F. J. and Lelieveld , J . 1997 . Radiative forcing due to tropospheric ozone and sulf-ate aerosols. J. Geophys. Res . 102 , D23, 28,079 - 28,100 .  

  46. Wadleigh , M. A. , Schwarcz , H. P. and Kramer , J. R . 1996 . Isotopic evidence for the origin of sulphate in coastal rain. Tellus 48B , 44 – 59 .  

  47. Xu , X . 1998 . Mass independent isotopic fractionation in solid phase. Ph.D. Dissertation , University of California, San Diego .  

comments powered by Disqus