收稿日期: 2010-04-16
修回日期: 2010-05-19
网络出版日期: 2011-04-10
Carbon Isotope Fractionation Mechanism of Alkane Gasesin Fischer-Tropsch Synthesis Experiments
Received date: 2010-04-16
Revised date: 2010-05-19
Online published: 2011-04-10
杨春, 王京红, 米敬奎, 高晓辉, 陶士振, 倪云燕, 陶小晚 . 费—托合成实验中烷烃气碳同位素分馏机理费—托合成实验中烷烃气碳同位素分馏机理[J]. 天然气地球科学, 2011 , 22(2) : 206 -210 . DOI: 10.11764/j.issn.1672-1926.2011.02.206
Fische-|Tropsch synthesis experiments indicate that carbon isotopes of alkane gases reversed in these experiments on occasion. By analyzing the whole process and data of all researchers,the probable interpretations are deduced as fellows. As the products conversion heightening with the experiment time and temperature increasing,the control of alkane carbon isotope fractionation in the experiments was gradually shifted from kinetic mechanism to thermodynamic equilibrium. Series of carbon isotopes of alkane gases were changed from reversed to normally distribution just like alkanes in natural gas. The experiments were controlled by kinetic fractionation on the conditions of short time reaction (low conversion) or in an opened system (discharging following the reaction). And the electric spark synthesis experiment was more an ideal condition delegating the course of carbon isotope fractionation.
[1]Anderson R B.The Fischer-Tropsch Synthesis[M].Newyork:Acdemia Press,1984:1-30.
[2]Zhou Lu.Study on Fischer-Tropsch synthesis reaction mechanism[J].Journal of Chengdu University of Science and Technology,1996,89(1):91-97.[周鲁.Fischer-Tropsch合成反应机理研究进展[J].成都科技大学学报,1996,89(1):91-97.]
[3]Lancet M S,Anders E.Carbon isotope fractionation in the Fischer-Tropsch synthesis and in meteorites[J].Science,1970,170 (3961):980-982.
[4]Anders E,Hayatsu R,Studier M H.Organic compounds in meteorites[J].Science,1973,182(4114):781-790.
[5]Hu G X,Ouyang Z Y.Carbon isotopic fractionation in the process of Fischer-Tropsch reaction in primitive solar nebula[J].Science in China:Series D,1998,41(2):202-207.[6]Horita J,Berndt M E.Abiogenic methane formation and isotopic fractionation under hydrothermal conditions[J].Science,1999,285(5430):1055-1057.
[7]McCollom T M,Seewald J S.Carbon isotope composition of organic compounds produced by abiotic synthesis under hydrothermal conditions[J].Earth and Planetary Science Letters,2006,243(1/2):74-84.
[8]Taran Yuri A,George A Kliger,Vyacheslav S Sevastianov.Carbon isotope effects in the open-system Fischer-Tropsch synthesis[J].Geochimica et Cosmochimica Acta,2007,71:4474-4487.
[9]Fu Q,Sherwood Lollar B,Horita J,et al.Abiogenic formation of hydrocarbons under hydrothermal conditions:Constraints from chemical and isotopic data[J].Geochimic Cosmochim Acta ,2007,71:1982-1998.
[10]Berndt M E,Allen D E,Seyfried W E.Reduction of CO2 during serpentinization of olivine at 300 degrees C and 500bar[J].Geology,1996,24(4):351-354.
[11]Sherwood Lollar B,Frape S K,Weise S M,et al.Abiogenic methanogenesis in crystalline rocks[J].Geochimica et Cosmochimica Acta,1993,57(23/24):5087-5097.
[12]Takahashi H,Liu L H,Yashiro Y,et al.CO2 reduction using hydrothermal method for the selective formation of organic compounds[J].Journal of Materials Science,2006,41(5):1585-1589.
[13]Dekov V.Native nickel in the TAG hydrothermal field sediments (Mid-Atlantic Ridge,26°N):Space trotter,guest from mantle,or a widespread mineral,connected with serpentinization[J].Journal of Geophysical Research,2006,111:1-9.
[14]McCollom T M,Seewald J S.A reassessment of the potential for reduction of dissolved CO2 to hydrocarbons during serpentinization of olivine[J].Geochimica et Cosmochimica Acta,2001,65:3769-3778.
[15]Foustoukos D I,Seyfried W E.Hydrocarbons in hydrothermal vent fluids:The role of chromium-bearing catalysts[J].Science,2004,304(5673):1002-1005.
[16]Giggenbach W F.Relative importance of thermodynamic and kinetic processes in governing the chemical and isotopic composition of carbon gases in high-heatflow sedimentary systems[J].Geochim Gosmochim Acta,1987,61:3763-3785.
[17]Fiebig J,Woodland A B,Spangenberg J,et al.Natural evidence for rapid abiogenic hydrothermal generation of CH4[J].Geochimica et Cosmochimica Acta,2007,71:3028-3039.
[18]Bottinga Y.Calculated fractionation factors for carbon and hydrogen isotope exchange in the system calcite-carbon dioxide-graphite-methane-hydrogen-water vapor[J].Geochimica et Cosmochimica Acta,1969,33:49-64.
[19]Schoell M.Genetic characterization of natural gases[J].American Association of Petroleum Geochemists Bulletin,1983,67:2225-2238.
[20]Abrajano T A,Sturchio N C,Bohlke J K,et al.Methane-hydrogen gas seeps,zambales ophiolite,philippines:Deep or shallow origin[J].Chemical Geology,1988,71(1/3):211-222.
[21]Zhu Zhimin,Shen Bing,Yan Jianfei.Discuss on inorganic natural gas in the Fuxin basin[J].Natural Gas Geoscience,2006,17(3):418-421.[朱志敏,沈冰,闫剑飞.阜新盆地无机成因气探讨[J].天然气地球科学,2006,17(3):418-421.]
[22]Galimov E M.Sources and formation mechanisms of hydrocarbon gases in sediments[J].Geochemistry International,1989,26:1-15.
[23]James A T,Correlation of natural gas by use of carbon isotope distribution between hydrocarbon components[J].AAPG Bulletin,1983,67(7):1176-1191.
[24]Dai Jinxing,Li Jian,Luo Xia,et al.Stable carbon isotope compositions and source rock geochemistry of the giant gas accumulations in the Ordos basin[J].China Organic Geochemistry,2005,36:1617-1635.
[25]Des Marais D J,Donchim J H,Nehring N L,et al.Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons[J].Nature,1981,292:826-828.
[26]Chung H M,Gorml J R,Squires R M.Origin of gaseous hydrocarbons in subsurface environments:Theoretic considerations of carbon isotope distribution[J].Chemical Geology,1988,71(1/3):97-104.
[27]Dai Jinxing.Composition characteristics and origin of carbon isotope of Liuhuangtang natural gas in Tengchong county,Yunnan province[J].Chinese Science Bulletin,1989,34(12):1027-1030.
[28]Dai Jinxing,Song Yan,Dai Chunsen,et al.Geochemistry and accumulation of carbon dioxide gases in China[J].AAPG Bulletin,1996,80(10):1615-1626.
[29]Dai Jinxing,Yang Shufeng,Chen Hanlin,et al.Geochemistry and occurrence of abiogenic gas accumulations in the Chinese sedimentary basins[J].Organic Geochemistry,2005,36:1664-1688.
[30]Dai Jinxing,Zou Caineng,Zhang Shuichang,et al.Discrimination of abiogenic and biogenic alkane gases[J].Science in China:Series D,2008,51(12):1737-1749.
[31]Hosgormez H,Yalcin M N,Cramer B,et al.Molecular and isotopic composition of gas occurrences in the Thrace basin (Turkey):Origin of the gases and characteristics of possible source rocks[J].Chemical Geology,2005,214:179-191.
[32]Sherwood Lollar B,Westgate T D,Ward J A,et al.Abiogenic formation of alkanes in the earth′s crust as a minor source for global hydrocarbon reservoirs[J].Nature,2002,416:522-524.
[33]Sherwood Lollar B,Lacrampe Couloume G,Slater G F,et al.Unravelling abiogenic and biogenic sources of methane in the earth′s deep subsurface[J].Chemical Geology,2006,226:328-339.
[34]Yuen G,Blair N,Des Marais D J,et al.Carbon isotope composition of low molecular weight hydrocarbons and monocarboxylic acids from murchison meteorite[J].Nature,1984,307:252-254.
[35]Yuen G U,Pecore J A,Kerridge J F,et al.Carbon isotope fractionation in Fischer-Tropsch type reactions[C].Lunar Planetary Science Conference XXI,1990:1367-1368.
[36]Wang Xianbin,Li Chunyuan,Chen Jianfa,et al.Discussion on abiogenic natural gases[J].Chinese Science Bulletin,1997,42(12):1233-1241.[王先彬,李春园,陈践发,等.论生物成因天然气[J],科学通报,1997,42(12):1233-1241.]
[37]Dai Jinxing.Characteristic of abiogenic gas resource and resource perspective[J].Natural Gas Geoscience,2006,17(1):1-6.[戴金星.非生物天然气资源的特征与前景[J].天然气地球科学,2006,17(1):1-6.]
[38]Galimov E M.Isotope organic geochemistry[J].Organic Geochemistry,2006,37:1200-1262.
/
〈 |
|
〉 |