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1 Journal of the Combustion Society of Japan Vol.56 No.176 (2014) ORIGINAL PAPER 半 導 体 レーザー 吸 収 分 光 法 の 自 動 車 排 気 中 の 二 酸 化 炭 素 炭 素 同 位 体 比 計 測 への 応 用 Application of Diode-laser Absorption Spectroscopy for Measurements of Stable Carbon Isotope Ratio of Carbon Dioxide in Automobile Exhaust 1 * * TANAKA, Kotaro 1 *, KOJIMA, Ryota 2, MIYAMURA, Kai 1, KONNO, Mitsuru 1, and TONOKURA, Kenichi 2 * Ibaraki University, Nakanarusawa, Hitachi, Ibaraki , Japan The University of Tokyo, Kashiwanoha, Kashiwa, Chiba , Japan ; Received 5 September, 2013; Accepted 16 December, 2013 Abstract : A high-sensitivity laser absorption spectroscopic technique has been employed for measurements of the stable carbon isotope ratio of carbon dioxide (CO 2), 13 CO 2/ 12 CO 2, in automobile exhaust. The amounts of 12 CO 2 and 13 CO 2 were detected through wavelength modulation spectroscopy using a distributed feedback laser diode in the 2-μm wavelength region. A 0.15-L one-pass optical cell with an effective optical path length of 0.5 m was used for continuous measurements of automobile exhaust, with the intention of maintaining the residence time to less than 5 s. In addition, a 0.9-L Herriott-type multi-pass optical cell with an effective optical path length of 29.9 m was used for precise measurements of the stable carbon isotope ratio of CO 2 in automobile exhaust, which was collected in a sampling bag. Continuous measurements of the stable carbon isotope ratio were performed with a reproducibility of 0.28 (1σ) in 14.8 % CO2 for every 1-s signal measurement without signal integration over an 1830 s period. The feasibility of the developed system was evaluated for continuous measurements of the CO 2 stable carbon isotope ratio in automobile exhaust. Resultantly, we successfully performed continuous measurements of the stable carbon isotope ratio of CO 2 in automobile exhaust and found that the stable carbon isotope ratio of CO 2 changed in accordance with the driving conditions. Key Words : Carbon dioxide, Stable carbon isotopes, Wavelength modulation spectroscopy, Near-IR, Exhaust 1. 緒 言 (CO2) IPCC ppm (parts per million mol/mol ) 379 ppm [1] CO2 13 CO2/ 12 CO2 ( ) CO2 [2] CO2 CO2 [3] * Corresponding author. tonokura@k.u-tokyo.ac.jp, k_tanaka@ mx.ibaraki.ac.jp [4] CO2 CO2 CO2 ( ) δ 13 C (1) Rsample 13 CO2/ 12 CO2 Rstandard 13 C/ 12 C [3] CO2 20 % [5] (72)
2 ~ ~ -50 [4] CO2 CO2 ( ) [6] CO [7] CO / (IRMS) [8,9] CO CO CO2 IRMS IRMS CO2 4.3 mm [10-16] 1.6 mm (DFB) CO2 [17-21] DFB (CRDS) [17] (WMS) [18-20] IRMS CO2 1.6 mm mm 2 mm DFB WMS Herriott [22-24] (424 ppmv, δ 13 C ) CO2 120 δ 13 C 0.02 [24] CO2 CO2 [23,24] WMS CO2 CO2 CO2 CO2 [7] CO2 CO2 CO2 2. 実 験 概 要 [23,24] WMS mm DFB (73)
![6 mm 100 2 mm 2 mm DFB WMS Herriott [22-24] (424 ppmv, δ 13 C -10.5 ) CO2 120 δ 13 C 0.](/docs-images/41/22670082/images/page_2.jpg "02 [24] CO2 CO2 [23,24] WMS CO2 CO2 CO2 CO2 [7] CO2 CO2 CO2 2. 実 験 概 要 [23,24] WMS 1 2.")
3 Table 1 Specification of the test gasoline vehicle. Fig.1 Schematic diagram of the experimental apparatus for the continuous measurements of CO2 stable carbon isotope ratios in automobile exhaust. M.C: Mass flow controller, P: Capacitance manometer. 500 mm 50 mm InGaAs Hz WMS khz ~ MHz 11 khz 2 AD PC CO2 12 CO cm -1 (2v1 + v2 l - v2 l + v3 R(17)e) 13 CO cm -1 (v1 + 2v2 l + v3 P(16)e) δ 13 C = % CO L JE [25] 10 m HEPA CO2 (δ 13 C = -29.7, CO2 concentration = 14.8 %) CO L 50 cm 29.9 m 16 ppb (parts per billion) CO2 % 50 cm 5.6 slm (standard liter per minute) 25 kpa Hz 313 K ± 0.1 K 20 % [26] 0.7 % WMS 12 CO2 13 CO2 12 CO2 13 CO % [24] L % ( 660 rpm (rounds per minute)) (74)
4 rpm (JIS 96 ) 30 CO2 503 K CO2 CO2 1 % 0.9 L 40 cm 29.9 m Herriott 313 K 10 kpa 100 CO rpm CO2 1/10 Fig.2 Signal intensity as a function of CO2 concentration. Line and circle markers: Low CO2 concentration. Dashed line and square markers: High CO2 concentration. Open markers: 12 CO2. Close markers: 13 CO2. 3. 結 果 および 考 察 3.1. 濃 度 較 正 と 再 現 性 の 評 価 0.15 L 0.9 L Herriott L CO2 0 ~ 20 % 0.9 L CO2 1 % 1/10 CO2 0 ~ 2 % 12 CO L 0.9 L 12 CO2 13 CO CO2 13 CO L Fig.3 Continuous measurements of CO2 stable carbon isotope ratio (δ 13 C = -29.7, CO2 concentration = 14.8 %) using a 0.15-L one-pass optical cell. δ 13 C = % CO Hz 1830 [25] 3 1σ 自 動 車 排 気 のリアルタイム 計 測 660 rpm 3000 rpm CO2 4 CO2 CO (75)
5 Table 2 CO2 concentrations and stable carbon isotope ratios in automobile exhaust. Fig.4 Continuous measurements of (a) stable carbon isotope ratios and (b) CO2 concentration in automobile exhaust. 2 mm CO 二 酸 化 炭 素 排 出 挙 動 と 炭 素 同 位 体 比 の 相 関 CO2 CO2 100 CO2 2 CO2 CO2 CO2 CO2 CO2 CO [7,27] CO CO2 13 C 12 C 12 C 13 C CO 13 CO 12 CO CO [5,6] 13 C [28] CO 12 C CO 12 C CO2 12 C 4. 結 言 2 mm DFB WMS CO2 CO2 % CO2 (76)
6 L ( 5 ) CO % (1σ) CO2 CO2 5 CO2 CO 12 C 謝 辞 References 1. IPCC Annual reports 4, Trudinger, C. M., Enting, I. G., Francey, R. J., Etheridge, D. M., and Rayner, P. J., Tellus 51B: (1999). 3. Hoefs, J., Stable isotope geochemistry 5th eds., Springer, (2004). 4. Pataki, D. E., Alig, R. J., Fung, A. S., Golubiewski, N. E., Kennedy, C. A., Mcpherson, E. G., Nowak, D. J., Pouyat, R. V. and Romerolankao, P., Global Change Biology 12: (2006). 5. National GHGs Inventory Report of Japan (2012) www-gio.nies.go.jp/aboutghg/nir/nir-e.html. (2012/2/25) 6. Tsunogai, U., Nakagawa, F., and Akiyama, K., NISSAN GLOBAL FOUNDATION report (in Japanese), nissan-zaidan.or.jp/membership/7405//upfiles/01052.pdf. (2012/2/25) 7. Tsunogai, U., Hachisu, Y., Komatsu, D. D., Nakagawa, F., Gamo, T., and Akiyama, K., Atmos. Environ. 37: (2003). 8. Chansai, S., Burch, R., Hardacre, C., Breen, J., and Meunier, F., J. Catal. 281: (2011). 9. Yang, Y., Disselkamp, R. S., Szanyi, J., Peden, C. H. F., Campbell, C. T., Goodwin Jr, J. G., Rev. Sci. Instrum. 77: (2006). 10. Weidmann, D., Wysocki, G., Oppenheimer, C., and Tittel, F. K., Appl. Phys. B 80: (2005). 11. McManus, J. B., Nelson, D. D., Shorter, J. H., Jimenez, R., Herndon, S., Saleska, S., and Zahniser, M., J. Modern. Optics 52: (2005). 12. Tuzson, B., Zeeman, M. J., Zahniser, M. S., and Emmenegger, L., Infrared Phys. Technol. 51: (2008). 13. Tuzson, B., Mohn, J., Zeeman, M. J., Werner, R. A., Eugster, W., Zahniser, M. S., Nelson, D. D., Mcmanus, J. B., and Emmenegger, L., Appl. Phys. B 92: (2008). 14. McManaus, J. B., Nelson, D. D., and Zahniser, M. S., Isot. Environ. Health Stud. 46: (2010). 15. Tuzson, B., Henne, S., Brunner, D., Steinbacher, M., Mohn, J., Buchmann, B., and Emmenegger, L., Atmos. Chem. Phys. Discuss. 11: (2011). 16. Wada, R., Pearce, J. K., Nakayama, T., Matsumi, Y., Hiyama, T., Inoue, G., and Shibata, T., Atmos. Environ. 45: (2011). 17. Wahl, E. H., Fidric, B., Rella, C. W., Koulikov, S., Kharlamov, B., Tan, S., Kachanov, A. A., Richman, B. A., Crosson, E. R., Paldus, B. A., Kalaskar, S., and Bowling, D. R., Isot. Environ. Health Stud. 42: (2006). 18. Gagliardi, G., Castrillo, A., Iannone, R. Q., Kerstel, E. R. T., and Gianfrani, L, Appl. Phys. B 77: (2003). 19. Castrillo, A., Casa, G., Burgel, M. V., Tedesco, D., and Gianfrani, L., Opt. Express 12: (2004). 20. Castrillo, A., Casa, G., Palmieri, A., and Gianfrani, L., Isot. Environ. Health Stud. 42: (2006). 21. Wehr, R., Kassi, S., Romanini, D., and Gianfrani, L., Appl. Phys. B 92: (2008). 22. Tanaka, K., and Tonokura, K. Appl. Phys. B 105: (2011). 23. Tanaka, K., Takahashi, K., and Tonokura, K., JSME Trans. B. (in Japanese) 78: (2012). 24. Tanaka, K., Kojima, R., Takahashi, K., and Tonokura, K., Infrared Phys. Technol. 60: (2013). 25. Ministry of Land, Infrastructure, Transport and Tourism (in Japanese) (2012/2/25) kijyun/saimokubetten/saibet_041_00.pdf. 26. Koike, S., Suzuki, H., Forum at National Traffic Safety and Environmental Laboratory (in Japanese). (2013/11/1) Kato, S., Akimoto, H., Braunlich, M., Rockmann, T., and Brenninkmeijer, Carl A. M., Geochem. J. 33 : (1999). 28. Akiyama, K., Proc. JSAE Annual Congress (Spring). (in Japanese) 79-12: (2012). (77)
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