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Title: Characterization of CO/sub 2/-CH/sub 4/-H/sub 2/O fluid inclusions by microthermometry and laser Raman microprobe spectroscopy: inferences for clathrate and fluid equilibria

Journal Article · · Geochim. Cosmochim. Acta; (United States)

Microthermometry (MT) and laser Raman microprobe (LRM) spectroscopy were done on 33 synthetically produced CO/sub 2/-CH/sub 4/-H/sub 2/O fluid inclusions in quartz. At room temperature, the inclusions consist of an aqueous liquid, a CO/sub 2/-CH/sub 4/ supercritical carbonic fluid, and graphite. In all these inclusions, the melting temperature for solid CO/sub 2/ is less than that for the homogenization of the vapor bubble in the carbonic fluid. A method is described whereby MT data for CO/sub 2/-CH/sub 4/-H/sub 2/O inclusions can be projected within the CO/sub 2/-CH/sub 4/ binary phase diagram to infer CO/sub 2/:CH/sub 4/ ratios in the carbonic fluid. This method takes into account the formation of CO/sub 2/-CH/sub 4/ clathrate hydrate during MT analysis. The authors interpretation of the MT data indicates that CH/sub 4/ is preferentially partitioned into the clathrate over the coexisting carbonic fluid, in contradiction to the prediction from PARRISH and PRAUSNITZ'S (1972) model for clathrate equilibria. Comparison of LRM analyses on the bulk carbonic fluid and the residual carbonic fluid confirm the preferential partitioning of CH/sub 4/ into the clathrate. LRM analyses of the clathrate itself indicate that CH/sub 4/ occupies both types of cage sites in the clathrate structure, whereas CO/sub 2/ may only occupy one site. Two by-products of the combined LRM and MT analyses of the same inclusions are derivation of empirical ratios of Raman quantification factors for high-density CO/sub 2/-CH/sub 4/ fluids and the ability to determine CO/sub 2/:CH/sub 4/ ratios of inclusions whose MT data lie near the critical region for CO/sub 2/-CH/sub 4/.

Research Organization:
Washington Univ., St. Louis, MO (USA)
OSTI ID:
7160170
Journal Information:
Geochim. Cosmochim. Acta; (United States), Vol. 51:6
Country of Publication:
United States
Language:
English

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