Kinetics of methane hydrate replacement with carbon dioxide and nitrogen gas mixture using in situ NMR spectroscopy

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DOIResolve DOI: http://doi.org/10.1021/es504888n
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TypeArticle
Journal titleEnvironmental Science & Technology
ISSN0013-936X
1520-5851
Volume49
Issue3
Pages19641971
AbstractIn this study, the kinetics of methane replacement with carbon dioxide and nitrogen gas in methane gas hydrate prepared in porous silica gel matrices has been studied by in situ ¹H and ¹³C NMR spectroscopy. The replacement process was monitored by in situ ¹H NMR spectra, where about 42 mol % of the methane in the hydrate cages was replaced in 65 h. Large amounts of free water were not observed during the replacement process, indicating a spontaneous replacement reaction upon exposing methane hydrate to carbon dioxide and nitrogen gas mixture. From in situ ¹³C NMR spectra, we confirmed that the replacement ratio was slightly higher in small cages, but due to the composition of structure I hydrate, the amount of methane evolved from the large cages was larger than that of the small cages. Compositional analysis of vapor and hydrate phases was also carried out after the replacement reaction ceased. Notably, the composition changes in hydrate phases after the replacement reaction would be affected by the difference in the chemical potential between the vapor phase and hydrate surface rather than a pore size effect. These results suggest that the replacement technique provides methane recovery as well as stabilization of the resulting carbon dioxide hydrate phase without melting.
Publication date
PublisherAmerican Chemical Society
LanguageEnglish
AffiliationMeasurement Science and Standards; Security and Disruptive Technologies; National Research Council Canada
Peer reviewedYes
NPARC number23000258
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Record identifier651bacd6-2106-4c16-b524-40ccf4ee7034
Record created2016-06-29
Record modified2016-07-08
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