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Characterization of Gas Generated by Sequential Hydrous Pyrolysis of Potential Gas-Prone Source Rocks for Tight-Gas Reservoirs in the Rocky Mountain Area

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Characterization of Gas Generated by Sequential Hydrous Pyrolysis of Potential Gas-Prone Source Rocks for Tight-Gas Reservoirs in the Rocky Mountain Area CHARACTERIZATION OF GAS GENERATED BY SEQUENTIAL HYDROUS PYROLYSIS OF POTENTIAL GAS-PRONE SOURCE ROCKS FOR TIGHT-GAS RESERVOIRS IN THE ROCKY MOUNTAIN AREA by Tingwei(Lucy) Ko ABSTRACT The source of unconventional gas in tight-gas reservoirs of the Rocky Mountain area is uncertain, but possible Cretaceous gas-prone source rocks include the Cameo coal zone, Mowry, Mancos, and Baxter/Hilliard Shales. Sequential hydrous pyrolysis experiments were conducted on immature samples of these source rocks to characterize their generated gases and evaluate their potential as sources for gas accumulations in the Greater Green River Basin and Piceance Basin. The experiments were conducted sequentially for 72 h at 300, 330, and 360°C, equivalent to measured vitrinite reflectance values of 1.0, 1.3, and 1.6 %Ro, respectively. After each 72 h experiment, the generated gas and expelled oil were removed from the reactor. Gases generated from each sequential experiment were analyzed for molecular composition and stable carbon and hydrogen isotopes. All source rocks generated significant hydrocarbon and non-hydrocarbon gases (N2, H2S, H2, and CO2). Cumulative yields of methane to butane increased with increasing thermal maturation. On a per gram of total-organic-carbon (TOC) basis, the methane yield from the Cameo coal at 360°C exceeded that at 300°C by almost eightfold. The cumulative methane yields on a TOC basis, from highest to lowest, are Cameo coal, Baxter/Hilliard, Mowry, and Mancos Shales. Cumulative gas wetness from both Mancos and Mowry Shales were high. With increasing thermal maturity, δ13C of methane from all four source rocks became lighter, consistent to the beginning trend of the convention model. The Baxter/Hillard Shale generated the greatest amount of H2, H2S, and CO2, on a TOC 13 basis, whereas Cameo coal generated the least. The relatively positive δ C values for CO2 from the Mancos Shale and Baxter Shale suggests it was sourced from thermal decomposition of 13 carbonate minerals in the original rock samples. More negative δ C values for CO2 from the 13 Cameo coal indicate that gas is from an organic source, while intermediate δ C of CO2 from the Mowry Shale indicates contributions from both organic and inorganic sources or merely from the inorganic source. Gases generated from laboratory experiments are isotopically lighter than gas sampled from the Jonah and Piceance Basin fields. Two explanations are proposed: 1) Migration effects from the source to the reservoir and escaping gas from reservoirs may significantly alter final gas iii compositions; 2) Gases from experiments only reach primary cracking stage of gas generation, whereas field gas may represent gas from secondary cracking of oils deeper in the basins. KEY WORDS: Carbon isotopes, natural gas, hydrous pyrolysis, Jonah Field, Piceance Basin iv TABLE OF CONTENTS ABSTRACT....................................................................................................................... iii LIST OF FIGURES ......................................................................................................... viii LIST OF TABLES.............................................................................................................xv LIST OF ABBREVIATIONS......................................................................................... xvii ACKNOWLEDGEMENTS........................................................................................... xviii CHAPTER 1 INTRODUCTION .........................................................................................1 1.1 Unconventional Tight Gas Resources............................................................................1 1.2 Research Objectives.......................................................................................................2 CHAPTER 2 PREVIOUS RESEACH.................................................................................5 2.1 The Process of Natural Gas Generation, from a Molecular Standpoint ........................5 2.2 Sources of Natural Gas and Their Genetic Isotopic Signatures...................................12 2.2.1 Source of Natural Gas in the Piceance Basin and Jonah Field..........................13 2.2.2 Implications of Carbon and Hydrogen Isotopes in Gases .................................15 2.2.3 Hydrogen Isotope Effects..................................................................................22 CHAPTER 3 GEOLOGICAL BACKGROUND ..............................................................25 3.1 Piceance Basin, Colorado ............................................................................................26 3.1.1 Source Rocks – Maturity and Potential.............................................................29 3.2 Greater Green River Basin, Wyoming.........................................................................35 3.2.1 Source Rocks – Maturity and Potential.............................................................40 CHAPTER 4 METHODS & EXPERIMENTS .................................................................47 4.1 Potential Source Rock Sample Collection ...................................................................47 4.2 Sources Rock Characterization....................................................................................49 4.2.1 Sample Analysis in the SRA .............................................................................50 4.3 Hydrous Pyrolysis Experiments...................................................................................55 4.3.1 Composite Sample Preparation .........................................................................56 4.3.2 Experimental Conditions...................................................................................57 4.3.3 Hydrocarbon Collection ....................................................................................57 4.4 Measured Vitrinite Reflectance ...................................................................................58 4.4.1 Sample Preparation............................................................................................58 4.4.2 Measured Vitrinite Reflectance.........................................................................61 v 4.5 Gas-Chromatogram (GC) Analysis..............................................................................62 4.6 Gas Composition and Isotope Analysis .......................................................................62 4.6.1 Gas Isotope Analysis .........................................................................................63 CHAPTER 5 RESULTS....................................................................................................65 5.1 Core Description of the Mowry Shale Core ................................................................65 5.2 Original Samples – Organic Geochemical Analysis....................................................65 5.2.1 Organic Richness...............................................................................................65 5.2.2 Thermal Maturity...............................................................................................66 5.2.3 Organic Matter Type .........................................................................................67 5.3 Mature Samples after HP – Results of SRA ................................................................67 5.4 Hydrous Pyrolysis Experiments...................................................................................67 5.4.1 Thermal maturity ...............................................................................................79 5.4.2 Gas Chromatograms of Expelled Oils...............................................................79 5.4.3 Gas Yields & Their Bulk Molecular Composition............................................86 5.4.3.1 The Bulk Yields.....................................................................................86 5.4.3.2 Hydrocarbon Gas Compositions and Gas Dryness ...............................92 5.4.3.3 CO2 and H2S..........................................................................................93 5.4.4 Non-hydrocarbon Gases ....................................................................................93 5.4.5 Eh & pH of the Recovered Water......................................................................97 5.4.6 Isotopic Composition of Natural Gas................................................................98 CHAPTER 6 DISCUSSION............................................................................................104 6.1 Mass Balance .............................................................................................................104 6.2 Kerogen Cracking Products and Products Yield .......................................................105 6.2.1 Hydrocarbon Gas Yields in Jonah Field & Southern Piceance Basin .............105 6.2.2 Bulk Compositions of Hydrocarbon Gases .....................................................109 6.2.3 Controls on Gas Generation Products and Their Yields .................................111 6.3 Non-hydrocarbon Gases.............................................................................................111 6.4 Eh & pH of the Recovered Water..............................................................................123 6.5 Gas: Oil Ratio (GOR) ................................................................................................124 6.6 The Relationship among Stable Isotopes, Kerogen Types, and Thermal Maturity...125
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