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• W4386566088 endingPage "123380" @default.
• W4386566088 startingPage "123380" @default.
• W4386566088 abstract "In recent years, increasing attention has been given to quantifying the isotopic compositions of gases by Raman spectroscopy. However, related research on the carbon isotopes of CH4 is still lacking. In this study, the Raman spectral characteristics of 13CH4 and 12CH4 in the pure CH4 system and in the CH4-H2O system are comprehensively studied at temperatures ranging from 25 to 400 °C and pressures ranging from 50 to 400 bar. For the pure CH4 system, the peak positions of the symmetric stretching band (ν1) of 13CH4 and 12CH4 both shift to a higher wavenumber with increasing temperature and decreasing pressure, and their full width at half maximum (FWHM) values can reach 4.7 cm-1 and 5.5 cm-1, respectively, with increasing temperature and density. The peak position of the ν1 band of 13CH4 is always 4.6-5.1 cm-1 lower than that of 12CH4 under the same conditions, indicating that 13CH4 and 12CH4 can be distinguished by peak position and FWHM in the Raman spectra. Although the calculated Raman shifts (ν0) at zero-density for 13CH4 and 12CH4 are different, the unified equation for determining the density of CH4-rich fluid inclusions is still applicable, as long as to bracket the sample measurement with measurements of reference standards. For the CH4-H2O system, the peak position of the ν1 band of dissolved 13CH4 is approximately 2.5 cm-1 lower than that of 12CH4, while their FWHM values can be more than 12.2 cm-1, causing more difficulty in distinguishing them in aqueous solutions. In addition, Raman quantitative calibration models of 12CH4 and 13CH4 in the CH4-H2O system are established. The difference in the Raman scattering cross section (RSCS) of dissolved 12CH4 and 13CH4, rather than changes in the molar density or RSCS of water is the main reason leading to the difference in the Raman quantitative calibration models of CH4 concentrations between the 12CH4-H2O system and the 13CH4-H2O system. Our work provides a good reference for the in situ identification and quantification of the carbon isotopic composition of CH4 in high-temperature and high-pressure environments." @default.
• W4386566088 created "2023-09-10" @default.
• W4386566088 creator A5000637378 @default.
• W4386566088 creator A5007307935 @default.
• W4386566088 creator A5015191692 @default.
• W4386566088 creator A5036011433 @default.
• W4386566088 creator A5050562110 @default.
• W4386566088 creator A5054493223 @default.
• W4386566088 date "2024-01-01" @default.
• W4386566088 modified "2023-10-15" @default.
• W4386566088 title "Comparison of Raman spectral characteristics and quantitative methods between 13CH4 and 12CH4 from 25 to 400 °C and 50 to 400 bar" @default.
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