A High-precision Measurement System for Carbon and Hydrogen Isotopic Ratios of Atmospheric Methane and Its Application to Air Samples Collected in the Western Pacific Region

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In order to study temporal and spatial variations of atmospheric CH_4 quantitatively, we originally improved a measurement system for carbon and hydrogen isotopic ratios (δ^<13>C and δD) of CH_4 to attain high-precision measurements. By analyzing 100mL aliquots of an ambient air sample, the precision of our system is 0.08‰ for δ^<13>C and 2.2‰ for δD (1σ), which are one of the highest precisions reported so far. The system consists mainly of a CH_4 preconcentration device and a continuous-flow gas chromatograph isotope ratio mass spectrometer equipped with a combustion furnace and a pyrolysis furnace for measurements of δ^<13>C and δD. The preconcentration trap temperature was maintained at -130±1℃ during collection of CH_4 from the air sample by passing it through the trap, then at -83±1℃ while remaining air components such as N_2 and O_2 except for CH_4 escaped, and finally at 100±1℃ for CH_4 elusion. The isotopic values are measured on a mass spectrometer, relative to respective reference gases. For this study, the δ^<13>C and δD values of the reference gases were calibrated against our primary standards provided by the IAEA: our δ^<13>C primary standard is NBS18, whereas our δD primary standards are V-SMOW and SLAP. To ensure the long-term stability and reproducibility of our measurement system, a calibrated whole air stored in a high-pressure cylinder, which was called "test gas," was measured at least twice on each day when sample measurements were made. To measure small air samples, such as those extracted from ice cores, we also examined the relation between the sample size and the measured value of δ^<13>C and δD: gradual enrichment of the δ^<13>C occurred with decreasing CH_4 content less than 8nmol whereas no such effect could be seen for the δD. Furthermore, preliminary results of latitudinal distributions of δ^<13>C and δD were discussed along with CH_4 concentrations obtained by our shipboard air-sampling program.
2009-06-25

A High-precision Measurement System for Carbon and Hydrogen Isotopic Ratios of Atmospheric Methane and Its Application to Air Samples Collected in the Western Pacific Region

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