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In Situ Fourier Transform Infrared Diffuse Reflectance and Photoacoustic Spectroscopy Characterization of Sulfur-Oxygen Species Resulting from the Reaction of SO2 with CaCO3

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Abstract:

Fourier transform photoacoustic and diffuse reflectance spectroscopies (FT-IR-PAS and -DRS) have been used in situ to monitor the reaction of SO2 (1.5% in N2) with particulate CaCO3 at temperatures up to 400°C (PAS) and 690°C (DRS). The PA spectra indicate that at 360°C SO2 is physisorbed on the CaCO3 surface. This species is readily desorbed by N2 purging. Under continuous SO2/N2 exposure at 400°C and above, the physisorbed species is shown by the DR data to be converted first to oxygen-bound and then to nonspecifically bound pyramidal SO3 Reaction of the SO3 with SO2 to form SO4 begins at 400°C and is essentially complete at 690°C. The DR data further indicate that for the SO4 : (1) at temperatures between 400 and 640°C a monodentate C species forms; (2) above 640°C the SO4 ion has nearly Td symmetry; and (3) upon subsequent cooling, the SO4 exhibits the characteristics of a chelating C species.

Keywords: Analysis for sulfur-oxygen species; Diffuse reflectance spectroscopy; Fourier transform infrared spectroscopy; Photoacoustic spectroscopy

Document Type: Research Article

DOI: http://dx.doi.org/10.1366/0003702884430155

Affiliations: P. M. Gross Chemistry Laboratory, Duke University, Durham, North Carolina 27706

Publication date: August 1, 1988

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