Chiang Wei-Shan, Chen Jin-Hong, Jacobi David, Yildirim Taner, Turkoglu Danyal, Althaus Stacey, Liu Yun
Aramco Services Company: Aramco Research Center-Houston, Texas, USA.
Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland, USA.
Energy Fuels. 2020;34(10). doi: 10.1021/acs.energyfuels.0c02268.
The thermogenic transformation of kerogen into hydrocarbons accompanies the development of a pore network within the kerogen that serves as gas storage locations both in pore space and surface area for adsorbed gas within the source rock. Therefore, the successful recovery of gas from these rocks depends on the accessible surface area, surface properties, and interconnectivity of the pore system. These parameters can be difficult to determine because of the nanoscale of the structures within the rock. This study seeks to investigate the pore structure, surface heterogeneity, and composition of recovered kerogens isolated from source rocks with progressively increasing thermogenic maturities. Prompt gamma-ray activation analysis (PGAA), nitrogen and methane volumetric gas sorption, and small-angle neutron scattering (SANS) are combined to explore the relationship between the chemical composition, pore structure, surface roughness, surface heterogeneity, and maturity. PGAA results indicate that higher mature kerogens have lower hydrogen/carbon ratio. Nitrogen gas adsorption indicates that the pore volume and accessible specific surface area are higher for more mature kerogens. The methane isosteric heat at different methane uptake in the kerogens is determined by methane isotherms and shows that approximately two types of binding sites are present in low mature kerogens while the binding sites are relatively homogeneous in the most mature kerogen. The hysteresis effect of the structure during the adsorption and desorption process at different CD gas pressures are studied. An extended generalized Porod's scattering law method (GPSLM) is further developed here to analyze kerogens with fractal surfaces. This extended GPSLM quantifies the surface heterogeneity of the kerogens with a fractal surface and shows that kerogen with high maturity is chemically more homogeneous, consistent with the results from methane isosteric heat. SANS analysis also suggests a pronounced surface roughness in the more mature kerogens. A microporous region circling around the nanopores, which contributes to high surface roughness and methane storage, is shown to develop with maturity.
干酪根向烃类的热成因转化伴随着干酪根内部孔隙网络的发育,该孔隙网络在孔隙空间以及烃源岩内吸附气体的表面积中均充当气体储存位置。因此,从这些岩石中成功开采天然气取决于孔隙系统的可及表面积、表面性质和连通性。由于岩石内部结构的纳米尺度,这些参数可能难以确定。本研究旨在研究从热成因成熟度逐渐增加的烃源岩中分离出的回收干酪根的孔隙结构﹑表面非均质性和组成。将瞬发伽马射线活化分析(PGAA)、氮气和甲烷体积气体吸附以及小角中子散射(SANS)相结合,以探究化学成分、孔隙结构、表面粗糙度、表面非均质性和成熟度之间的关系。PGAA结果表明,成熟度较高的干酪根具有较低的氢碳比。氮气吸附表明,成熟度较高的干酪根的孔隙体积和可及比表面积更大。通过甲烷等温线确定了干酪根中不同甲烷吸附量下的甲烷等量吸附热,结果表明,低成熟度干酪根中存在大约两种类型的结合位点,而在最成熟的干酪根中结合位点相对均匀。研究了不同CD气体压力下吸附和解吸过程中结构的滞后效应。在此进一步开发了一种扩展的广义Porod散射定律方法(GPSLM),用于分析具有分形表面的干酪根。这种扩展的GPSLM量化了具有分形表面的干酪根的表面非均质性,结果表明,成熟度高的干酪根在化学上更均匀,这与甲烷等量吸附热的结果一致。SANS分析还表明,成熟度较高的干酪根具有明显的表面粗糙度。结果显示,随着成熟度的增加,围绕纳米孔形成了一个微孔区域,这导致了高表面粗糙度和甲烷储存。