Journal
JOURNAL OF RAMAN SPECTROSCOPY
Volume 52, Issue 3, Pages 750-769Publisher
WILEY
DOI: 10.1002/jrs.6033
Keywords
Attraction; Fugacity; Molar volume; Repulsion
Categories
Funding
- University of Potsdam
- NSERC
- University of Missouri
- National Science Foundation [EAR-1624589, OCE-1459433]
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The Raman spectral behavior of N-2, CO2, and CH4 in ternary N-2-CO2-CH4 mixtures was studied, with N-2 showing lower wavenumbers in all mixtures, while CO2 and CH4 exhibited different peak shifts. The relationships between peak positions and mole fractions were found to be more complex for CH4 compared with N-2 and CO2. Additionally, the study extended the relationship between the peak position of N-2 and pressure in ternary N-2-bearing systems to assess similarities in Raman spectral behavior.
The Raman spectral behavior of N-2, CO2, and CH4 in ternary N-2-CO2-CH4 mixtures was studied from 22 degrees C to 200 degrees C and 10 to 500 bars. The peak position of N-2 in all mixtures is located at lower wavenumbers compared with pure N-2 at the same pressure (P)-temperature (T) (PT) conditions. The Fermi diad splitting in CO2 is greater in the pure system than in the mixtures, and the Fermi diad splitting increases in the mixtures as CO2 concentration increases at constant P and T. The peak position of CH4 in the mixtures is shifted to higher wavenumbers compared with pure CH4 at the same PT conditions. However, the relationship between peak position and CH4 mole fraction is more complicated compared with the trends observed with N-2 and CO2. The relative order of the peak position isotherms of CH4 and N-2 in the mixtures in pressure-peak position space mimics trends in the molar volume of the mixtures in pressure-molar volume space. Relationships between the direction of peak shift of individual components in the mixtures, the relative molar volumes of the mixtures, and the attraction and repulsion forces between molecules are developed. Additionally, the relationship between the peak position of N-2 in ternary N-2-CO2-CH4 mixtures with pressure is extended to other N-2-bearing systems to assess similarities in the Raman spectral behavior of N-2 in various systems.
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