The shale gas potential of Ediacaran and Lower Silurian shales from the Upper Yangtze platform is assessed in this study with a focus on the contributions of clay minerals and organic matter to sorption capacity. For this purpose, a multidisciplinary assessment was carried out using petrophysical, mineralogical, petrographic and geochemical methods. In terms of TOC contents (4.2%), brittle mineral contents (68.6%) and maximum gas storage capacities (0.054–0.251 mmol/g) Ediacaran shales from this study show comparable properties to other producing shale gas systems although the thermal maturity is extremely high (VRr = 3.6%). When compared to lower Silurian shales from the same region, it is evident that (1) deeper maximum burial and (2) a lack of silica-associated preservation of the pores resulted in a relatively lower mesopore volume, higher micropore volume fraction and lower overall porosity (Ediacaran shales: 1.4–4.6%; Silurian shales: 6.2–7.4%). Gas production is therefore retarded by poor interconnectivity of the pore system, which was qualitatively demonstrated by comparing experimental gas uptake kinetics. TOC content exhibits a prominent control on sorption capacity and micropore volume for both shales. However, different contributions of clay minerals to sorption capacity were identified. This can partly be attributed to different clay types but is likely also related to burial-induced recrystallisation and different origins of illite. Additionally, it was shown that variations in sorption capacity due to incorrect estimates of clay mineral contribution are in the same range as variations due to differences in thermal maturity.
Article highlights
Pore structure and gas storage characteristics are evaluated for the first time for Ediacaran Shales from the Upper Yangtze platform
Due to a lower free gas storage capacity and diffusivity, the Ediacaran shale can be regarded as a less favorable shale gas prospect when compared to the Silurian shale
Clay mineral contribution to sorption capacity is evaluated taking clay mineralogy into consideration
Maturity-related changes of organic matter sorption capacity have been discussed on the basis of a compiled data set
Crushing and grinding of carbonaceous shale samples is likely to enhance the accessibility of pores and embedded organic matter as compared to the intact rock. This may lead to an overestimation of the total (volume and sorptive) gas storage capacity. In order to investigate the importance of these effects we have measured unconfined apparent grain densities (helium pycnometry) and methane sorption capacities (high-pressure methane excess sorption) of four carbonaceous shales (Cambro-Ordovician Alum Shale, Jurassic Kimmeridge Clay, Jurassic/Cretaceous Bazhenov Shale, and Late Cretaceous Eagle Ford Shale) as a function of particle size. Measurements were first conducted on 38 mm diameter core plugs, which then were crushed and milled to successively smaller particle sizes (<10 mm, <2 mm, <64 μm, and <1 μm). Apparent grain densities of the smallest particle fractions of the Alum, Bazhenov and Kimmeridge samples were consistently higher by 0.5 to 1% than apparent grain densities of the original sample plugs. Methane excess sorption capacity increased significantly for particle sizes <64 μm for the Alum and <1 μm for the Bazhenov and Kimmeridge samples while no significant changes upon grinding were observed for the Eagle Ford Shale. For the Bazhenov Shale, the apparent grain density increased slightly from 2.446 g/cm3 to 2.450 g/cm3 upon particle size reduction from <64 μm to <1 μm while the maximum sorption capacity (“Langmuir volume”) increased substantially from 0.11 mmol/g to 0.19 mmol/g. Similarly, for the Kimmeridge Clay and Alum Shale, a slight increase of the apparent grain density from 1.546 g/cm3 to 1.552 g/cm3 and from 2.362 g/cm3 to 2.385 g/cm3, respectively, was accompanied by increases in sorption capacity from 0.37 mmol/g to 0.45 mmol/g and from 0.14 mmol/g to 0.185 mmol/g, respectively. The increase in sorption capacity indicates an opening of a considerable amount of micropores with large internal surface area upon physical disruption of the rock fabric and/or removal of included fluids. It may also be due to increased swelling abilities of clay minerals and organic matter upon destruction of the stabilizing rock fabric with decreasing particle size. Grain density and sorption isotherms measured on small particle sizes are likely to overestimate the gas storage capacities and the amounts of producible gas-in-place since under field conditions (largely undisrupted rock fabric), significant portions of this storage capacity are essentially inaccessible. Poor interconnectivity of the pore system and slow, diffusion-controlled transport will massively retard gas production. Based on these findings, particle sizes >64 μm should be used for porosity and sorption measurements because they are more likely to retain the properties of the rock fabric in terms of accessible pore volume and sorptive storage capacity.
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