A thermodynamic investigation of adsorbate‐adsorbate interactions of carbon dioxide on nanostructured carbons

Murialdo, Maxwell; Ahn, Channing C.; Fultz, B.

doi:10.1002/aic.15996

Cited by 11 publications

(8 citation statements)

References 51 publications

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“…Smaller CO 2 and CH 4 uptakes are observed for IMt-2, reflecting its smaller total pore volume. However, the large fraction of micropores of IMt-2 results in a steep initial increase of the measured isotherms that is indeed typical of microporous materials. ,− Interestingly, the isotherms of IMt-2 also show moderate, but not negligible, hystereses for both CO 2 and CH 4 at all temperatures. Previous observations of hysteresis at supercritical conditions have been limited to swelling clay minerals, such as smectite, , the microstructure of which is sensitive to the water content .…”

Section: Resultsmentioning

confidence: 90%

“…|∆h| increases as a function of loading by approximately 5 to 6 kJ/mol and 3 to 4 kJ/mol for CO 2 and CH 4 , respectively. This behavior is the result of increasing lateral adsorbate interactions on relatively homogeneous surfaces73,82,83 of clay minerals as opposed to heterogeneous shales that show decreasing |∆h| for CO 2 and CH 4 84. s t e r i c e n t h a l p y , ∆h [ k J / m o l ] E x c e s s a m o u n t , n e x [ ‫؍‬ m o l / g ]…”

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confidence: 99%

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Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals

Hwang

Pini

2019

Environ. Sci. Technol.

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Clay minerals abound in sedimentary formations and the interaction of reservoir gases with their sub-micron features has direct relevance to many geo-energy applications. The quantification of gas uptake over a broad range of pressures is key towards assessing the significance of these physical interactions on enhancing storage capacity and gas recovery. We report a systematic investigation of the sorption properties of three source clay minerals-Na-rich montmorillonite (SWy-2), illite-smectite mixed layer (ISCz-1), and illite (IMt-2)-using CO 2 and CH 4 up to 30 MPa at 25 to 115 • C. The textural characterization of the clays by gas physisorption indicates that micropores are only partly accessible to N 2 (77 K) and Ar (87 K), while larger uptakes are measured with CO 2 (273 K) in the presence of illite. The supercritical excess sorption experiments confirm these findings, while revealing differences in uptake capacities that originate from the clay-specific pore size distribution. The Lattice Density Functional Theory (LDFT) model describes accurately the measured sorption isotherms by using a distribution of properly weighted slit pores and clay-specific solid-fluid interaction energies, which agree with isosteric heats of adsorption obtained experimentally. The model indicates that the maximum degree of pore occupancy is universal to the three 1 clays and the two gases, and it depends solely on temperature, reaching values near unity at the critical temperature. These observations greatly support the model's predictive capability for estimating gas adsorption on clay-bearing rocks and sediments.

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Section: Resultsmentioning

confidence: 90%

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confidence: 99%

Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals

Hwang

Pini

2019

Environ. Sci. Technol.

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“…However, lateral interactions between hydrogen molecules and cooperative adsorption could also play an important role. The increase of Q st,exc with θ has also been observed for other gases, such as water [91], ethane [59], carbon dioxide [92,93] and methane [58]. Torres-Knopp et al [94] found that lateral interactions between hydrogen molecules and cooperative adsorption lead to an increase of Q st with θ.…”

Section: Isosteric Heat Of Adsorptionmentioning

confidence: 77%

Application of the modified Dubinin-Astakhov equation for a better understanding of high-pressure hydrogen adsorption on activated carbons

Sdanghi

Schaefer

Maranzana

et al. 2020

International Journal of Hydrogen Energy

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Hydrogen storage in activated carbons (ACs) has proven to be a realistic alternative to compression and liquefaction. Adsorption capacities up to 5.8 wt.% have indeed been obtained. The amount of adsorbed hydrogen depends on the textural properties of ACs, such as specific surface area and total pore volume. The modified Dubinin-Astakhov (MDA) equation proved to be a good analytical tool for describing hydrogen adsorption in a wide range of pressures and temperatures and for several adsorbents. The parameters of this model have been found to be somehow related to the textural properties of the adsorbent. Thus, we applied this model to understand better hydrogen adsorption on ACs over a wide range of pressures in relation to the textural properties of the ACs. We applied the MDA equation to evaluate also the isosteric heat of hydrogen adsorption, which was found to be in the range of 5 to 9 kJ mol-1. We compared the results obtained by applying the MDA equation with those obtained by both the sorption isosteric method and the Sips equation. This allowed finding the temperature dependence of the isosteric heat of adsorption, as well as its variation with respect to the textural properties of the ACs.

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“…The standard state usually refers to the liquid-like state of gas for subcritical gas adsorption processes, however, this assumption is not valid for supercritical fluids (Zhou et al, 2000a(Zhou et al, & 2000bZhou et al, 2009). Moreover, using the liquid methane density or quasi-liquid density to extrapolate the absolute adsorption uptake from directly measured data is questionable even though previous works assert that the assumption allows researchers to investigate adsorption thermodynamics by considering both real gas behavior and the effect of adsorbed phase (Mertens et al, 2009;Stadie et al, 2013;Stadie et al, 2015;Tang et al, 2017aTang et al, , 2017bTang et al, & 2017cMurialdo et al, 2018). As mentioned earlier, the liquid methane density or quasi-liquid assumption contradicts molecular dynamics simulations where adsorbed density is a function of pressure and temperature.…”

Section: Introductionmentioning

confidence: 99%

New perspectives on supercritical methane adsorption in shales and associated thermodynamics

Tang

Ripepi

Rigby

et al. 2019

Journal of Industrial and Engineering Chemistry

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A thermodynamic investigation of adsorbate‐adsorbate interactions of carbon dioxide on nanostructured carbons

Cited by 11 publications

References 51 publications

Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals

Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals

Application of the modified Dubinin-Astakhov equation for a better understanding of high-pressure hydrogen adsorption on activated carbons

New perspectives on supercritical methane adsorption in shales and associated thermodynamics

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A thermodynamic investigation of adsorbate‐adsorbate interactions of carbon dioxide on nanostructured carbons

Cited by 11 publications

References 51 publications

Supercritical CO2 and CH4 Uptake by Illite-Smectite Clay Minerals

Supercritical CO2 and CH4 Uptake by Illite-Smectite Clay Minerals

Application of the modified Dubinin-Astakhov equation for a better understanding of high-pressure hydrogen adsorption on activated carbons

New perspectives on supercritical methane adsorption in shales and associated thermodynamics

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Product

Resources

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Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals

Supercritical CO₂ and CH₄ Uptake by Illite-Smectite Clay Minerals