成熟度不同的干酪根的结构性质,Energy & Fuels

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成熟度不同的干酪根的结构性质
Energy & Fuels ( IF 5.2 ) Pub Date : 2020-09-21 , DOI: 10.1021/acs.energyfuels.0c02268
Wei-Shan Chiang _{1,

2,

3} , Jin-Hong Chen ₁ , David Jacobi ₁ , Taner Yildirim ₂ , Danyal Turkoglu ₂ , Stacey Althaus ₁ , Yun Liu _{2,

3}

Affiliation

干酪根向烃的热转化伴随着干酪根内孔隙网络的发展，该孔隙网络既用作孔隙空间又用作吸附烃源岩的表面积的气体储存位置。因此，从这些岩石中成功回收气体取决于可及的表面积，表面性质和孔隙系统的互连性。由于烃源岩内部结构的纳米尺度，这些参数可能难以确定。这项研究旨在调查孔隙度，表面非均质性和分离的干酪根的组成，并逐渐增加来自中东储层烃源岩的生热成熟度。快速的伽马射线活化分析（PGAA），氮气和甲烷的体积气体吸附，结合小角度中子散射（SANS）来探讨化学成分，孔隙结构，表面粗糙度，表面不均匀性和成熟度之间的关系。PGAA结果表明，更成熟的干酪根具有较低的氢/碳比。氮气吸附表明，较成熟的干酪根的孔体积和可及的比表面积较高。甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在不太成熟的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一。结构在不同CD吸附和解吸过程中的磁滞效应孔隙结构，表面粗糙度，表面异质性和成熟度。PGAA结果表明，更成熟的干酪根具有较低的氢/碳比。氮气吸附表明，较成熟的干酪根的孔体积和可及的比表面积较高。甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在不太成熟的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一。结构在不同CD吸附和解吸过程中的磁滞效应孔隙结构，表面粗糙度，表面异质性和成熟度。PGAA结果表明，更成熟的干酪根具有较低的氢/碳比。氮气吸附表明，较成熟的干酪根的孔体积和可及的比表面积较高。甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在不太成熟的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一。结构在不同CD吸附和解吸过程中的磁滞效应氮气吸附表明，较成熟的干酪根的孔体积和可及的比表面积较高。甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在不太成熟的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一。结构在不同CD吸附和解吸过程中的磁滞效应氮气吸附表明，较成熟的干酪根的孔体积和可及的比表面积较高。甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在较不成熟的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。结构在不同CD吸附和解吸过程中的磁滞效应甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在较不成熟的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。结构在不同CD吸附和解吸过程中的磁滞效应甲烷等温线确定了干酪根中不同甲烷吸收量下的甲烷等排热，表明在较不成熟的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。结构在不同CD吸附和解吸过程中的磁滞效应_{研究了4种}气压。此处进一步扩展了扩展的广义Porod散射定律方法（GPSLM），以分析具有分形表面的干酪根。扩展的GPSLM定量分析了具有分形表面的干酪根的表面异质性，并表明更成熟的干酪根在化学上更均一，这与甲烷等温热的结果一致。SANS分析还表明，较成熟的干酪根具有明显的表面粗糙度。显示出围绕纳米孔的微孔区域随着成熟而发展，这有助于高表面粗糙度和甲烷存储。

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Structural Properties of Kerogens with Different Maturities

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 the surface area for adsorbed gas with source rocks. 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 source rocks. This study seeks to investigate the pore structure, surface heterogeneity, and composition of isolated kerogens with progressively increasing thermogenic maturities from source rocks at a middle-east reservoir. 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 more mature kerogens have lower hydrogen/carbon ratios. 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 uptakes in the kerogens is determined by methane isotherms and shows that approximately two types of binding sites are present in less mature kerogens while the binding sites are relatively homogeneous in the most mature kerogen. The hysteresis effects of the structure during the adsorption and desorption processes at different CD₄ 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 more mature kerogen 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.

更新日期：2020-10-16

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