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DOI | 10.1073/pnas.1906507117 |
Isotopic evidence for quasi-equilibrium chemistry in thermally mature natural gases | |
Thiagarajan, Nivedita1; Xie, Hao1; Ponton, Camilo2; Kitchen, Nami1; Peterson, Brian3; Lawson, Michael4; Formolo, Michael5; Xiao, Yitian5; Eiler, John1 | |
2020-02-25 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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ISSN | 0027-8424 |
出版年 | 2020 |
卷号 | 117期号:8页码:3989-3995 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | Natural gas is a key energy resource, and understanding how it forms is important for predicting where it forms in economically important volumes. However, the origin of dry thermogenic natural gas is one of the most controversial topics in petroleum geochemistry, with several differing hypotheses proposed, including kinetic processes (such as thermal cleavage, phase partitioning during migration, and demethylation of aromatic rings) and equilibrium processes (such as transition metal catalysis). The dominant paradigm is that it is a product of kinetically controlled cracking of longchain hydrocarbons. Here we show that C2+ n-alkane gases (ethane, propane, butane, and pentane) are initially produced by irreversible cracking chemistry, but, as thermal maturity increases, the isotopic distribution of these species approaches thermodynamic equilibrium, either at the conditions of gas formation or during reservoir storage, becoming indistinguishable from equilibrium in the most thermally mature gases. We also find that the pair of CO2 and C-1 (methane) exhibit a separate pattern of mutual isotopic equilibrium (generally at reservoir conditions), suggesting that they form a second, quasi-equilibrated population, separate from the C-2 to C-5 compounds. This conclusion implies that new approaches should be taken to predicting the compositions of natural gases as functions of time, temperature, and source substrate. Additionally, an isotopically equilibrated state can serve as a reference frame for recognizing many secondary processes that may modify natural gases after their formation, such as biodegradation. |
英文关键词 | stable isotopes compound-specific isotope analysis clumped isotopes natural gas methane |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000516771500021 |
WOS关键词 | TRANSITION-METAL CATALYSIS ; METHANE CLUMPED ISOTOPES ; METASTABLE EQUILIBRIUM ; CARBON ; HYDROCARBONS ; GENERATION ; PYROLYSIS ; PETROLEUM ; CONSTRAINTS ; GEOCHEMISTRY |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/249601 |
专题 | 地球科学 |
作者单位 | 1.CALTECH, Dept Geol & Planetary Sci, Pasadena, CA 91125 USA; 2.Western Washington Univ, Geol Dept, Bellingham, WA 98225 USA; 3.ExxonMobil Corp Strateg Res, Annandale, NJ 08801 USA; 4.ExxonMobil Upstream Business Dev, Spring, TX 77389 USA; 5.ExxonMobil Upstream Res Co, Spring, TX 77389 USA |
推荐引用方式 GB/T 7714 | Thiagarajan, Nivedita,Xie, Hao,Ponton, Camilo,et al. Isotopic evidence for quasi-equilibrium chemistry in thermally mature natural gases[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2020,117(8):3989-3995. |
APA | Thiagarajan, Nivedita.,Xie, Hao.,Ponton, Camilo.,Kitchen, Nami.,Peterson, Brian.,...&Eiler, John.(2020).Isotopic evidence for quasi-equilibrium chemistry in thermally mature natural gases.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,117(8),3989-3995. |
MLA | Thiagarajan, Nivedita,et al."Isotopic evidence for quasi-equilibrium chemistry in thermally mature natural gases".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 117.8(2020):3989-3995. |
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