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Adsorption Equilibria and Systematic Thermodynamics Analysis of Carbon Dioxide Sequestration on South African Coals Using Nonlinear Three-Parameter Models: Sips, Tóth, and Dubinin–Astakhov
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Adsorption Equilibria and Systematic Thermodynamics Analysis of Carbon Dioxide Sequestration on South African Coals Using Nonlinear Three-Parameter Models: Sips, Tóth, and Dubinin–Astakhov
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Adsorption Equilibria and Systematic Thermodynamics Analysis of Carbon Dioxide Sequestration on South African Coals Using Nonlinear Three-Parameter Models: Sips, Tóth, and Dubinin–Astakhov
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Journal Article
Adsorption Equilibria and Systematic Thermodynamics Analysis of Carbon Dioxide Sequestration on South African Coals Using Nonlinear Three-Parameter Models: Sips, Tóth, and Dubinin–Astakhov
2025
Overview
Carbon dioxide (CO2) injection into geologic formations has gained global traction, including in South Africa, to mitigate anthropogenic emissions through carbon capture, utilisation, and storage technology. These technological and technical developments require a comprehensive and reliable study of CO2 sorption equilibria under in situ unmineable coal reservoir conditions. This paper presents novel findings on the study of the equilibrium adsorption of CO2 on two South African coals measured at four temperatures between 30 and 60 °C and pressures up to 9.0 MPa using the volumetric technique. Additionally, the sorption mechanism and thermodynamic nature of the process were studied by fitting the experimental data into Langmuir–Freundlich (Sips), Tóth, and Dubinin–Astakhov (DA) isotherm models, and the Clausius–Clapeyron equation. The findings indicate that the sorption process is highly exothermic, as presented by a negative temperature effect, with the maximum working capacity estimated to range between 3.46 and 4.16 mmol/g, which is also rank- and maceral composition-dependent, with high-rank vitrinite-rich coal yielding more sorption capacity than low-rank inertinite-rich coal. The experimental data fit well in Sips and Tóth models, confirming their applicability in describing the CO2 sorption behaviour of the coals under the considered conditions. The isosteric heat of adsorption varied from 7.518 to 37.408 kJ/mol for adsorbate loading ranging from 0.4 to 3.6 mmol/g. Overall, the coals studied demonstrate well-developed sorption properties that characteristically make them viable candidates for CO2 sequestration applications for environmental sustainability.
