Extraction of Hydrocarbons from High-Maturity Marcellus Shale Using Supercritical Carbon Dioxide

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• 作者：Palma J. Jarboe ; Philip A. Candela ; Wenlu Zhu ; Alan J. Kaufman
• 刊名：Energy & Fuels
• 出版年：2015
• 出版时间：December 17, 2015
• 年：2015
• 卷：29
• 期：12
• 页码：7897-7909
• 全文大小：855K
• ISSN：1520-5029

文摘

Shale is now commonly exploited as a hydrocarbon resource. Due to the high degree of geochemical and petrophysical heterogeneity both between shale reservoirs and within a single reservoir, there is a growing need to find more efficient methods of extracting petroleum compounds (crude oil, natural gas, bitumen) from potential source rocks. In this study, supercritical carbon dioxide (CO₂) was used to extract n-aliphatic hydrocarbons from ground samples of Marcellus shale. Samples were collected from vertically drilled wells in central and western Pennsylvania, USA, with total organic carbon (TOC) content ranging from 1.5 to 6.2 wt %. Extraction temperature and pressure conditions (80 掳C and 21.7 MPa, respectively) were chosen to represent approximate in situ reservoir conditions at sample depth (1920鈥?280 m). Hydrocarbon yield was evaluated as a function of sample matrix particle size (sieve size) over the following size ranges: 1000鈥?00 渭m, 250鈥?25 渭m, and 63鈥?5 渭m. Several methods of shale characterization including Rock-Eval II pyrolysis, organic petrography, Brunauer鈥揈mmett鈥揟eller surface area, and X-ray diffraction analyses were also performed to better understand potential controls on extraction yields. Despite high sample thermal maturity, results show that supercritical CO₂ can liberate diesel-range (n-C₁₁ through n-C₂₁) n-aliphatic hydrocarbons. The total quantity of extracted, resolvable n-aliphatic hydrocarbons ranges from approximately 0.3 to 12 mg of hydrocarbon per gram of TOC. Sieve size does have an effect on extraction yield, with highest recovery from the 250鈥?25 渭m size fraction. However, the significance of this effect is limited, likely due to the low size ranges of the extracted shale particles. Additional trends in hydrocarbon yield are observed among all samples, regardless of sieve size: 1) yield increases as a function of specific surface area (r² = 0.78); and 2) both yield and surface area increase with increasing TOC content (r² = 0.97 and 0.86, respectively). Given that supercritical CO₂ is able to mobilize residual organic matter present in overmature shales, this study contributes to a better understanding of the extent and potential factors affecting the extraction process.