CO<sub>2</sub> Solubility in Aqueous Electrolyte Solutions Confined in Calcite Nanopores

Ali, Azeezat; Striolo, Alberto; Cole, David R.

doi:10.1021/acs.jpcc.1c02219

Cited by 12 publications

(17 citation statements)

References 59 publications

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“…We acknowledge that the results in bulk solutions are not perfectly transferable to confined systems. Even though the overall fraction of water present in composites equilibrated at 100% RH ( vide infra ) is considerably lower than what we measured here in the bulk, it is known that confinement can, in some cases, change the solubility of small molecules relative to bulk solutions . However, the results are an important first step in quantifying the AIE response of THPE in humidified PEI.…”

Section: Resultscontrasting

confidence: 56%

“…Even though the overall fraction of water present in composites equilibrated at 100% RH (vide inf ra) is considerably lower than what we measured here in the bulk, it is known that confinement can, in some cases, change the solubility of small molecules relative to bulk solutions. 56 However, the results are an important first step in quantifying the AIE response of THPE in humidified PEI. Turning to confined systems, we then prepared a series of composite samples equilibrated for 72 h at different values of RH according to a procedure described in the Methods section.…”

Section: The Journal Of Physical Chemistry Cmentioning

confidence: 99%

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Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

et al. 2023

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Direct air capture (DAC) technology is being explored as a pathway for reducing greenhouse gas emissions through the efficient removal of CO2 from the atmosphere. However, there remains a knowledge gap regarding structure–property–performance factors that impact the behavior of these systems in diverse, real-world environments. In aminopolymer-based DAC systems, gas diffusion is tightly coupled with polymer mobility, which is in turn affected by a large matrix of variables, including interactions with the pore wall of the support, nanoconfinement, the presence of co-adsorbates (moisture), and electrostatic cross-links that develop as a function of CO2 chemisorption. Higher-throughput, benchtop techniques for studying and understanding mobility in these systems would lead to more rapid advances in the field. Here, we demonstrate the value of a fluorescence technique for monitoring polymer mobility within nanocomposite capture materials as a function of CO2 and water adsorption in a series of humidified polyethylenimine-Al2O3 composite materials. The approach allows us to correlate changes in mobility with CO2 adsorption kinetics as a function of relative humidity. We further couple this information with NMR relaxometry data attained using a portable single-sided magnetic resonance device, and we employ diffuse reflectance infrared Fourier transform spectroscopy to correlate the formation of different relative amounts of carbamates and carbonates with the environmental conditions. These results provide a blueprint for using benchtop techniques to promote fundamental understanding in DAC systems that can in turn enable more efficient operation in real-world conditions.

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Section: Resultscontrasting

confidence: 56%

Section: The Journal Of Physical Chemistry Cmentioning

confidence: 99%

Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

et al. 2023

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“…However, industry works exclusively with pressurized CO 2 (PCO 2 ) in capture, transport and storage. In many such cases, the CO 2 is in dissolved form (1 -110 bar) 13,14 . PCO 2 is also the e uent of various industrial processes, such as natural gas reforming and ethylene oxide production (3 -20 bar) 15,16 .…”

Section: Introductionmentioning

confidence: 99%

Pressure dependence in aqueous-based electrochemical CO2 reduction

Huang

Gao

Yang

et al. 2022

Preprint

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Electrochemical CO2 reduction (CO2R) is an approach to closing the carbon cycle for chemical synthesis. To date, the field has focused on the electrolysis of ambient pressure CO2. However, industrial CO2 is pressurized – in capture, transport and storage – and is often in dissolved form. Here, we discover that pressurization up to 50 bar steers CO2R pathways toward formate, as universally exemplified on common CO2R catalysts. By developing operando methods compatible with high pressures, including quantitative operando Raman spectroscopy, we ascribe the pronounced formate selectivity to the higher CO2* coverages and lower hydronium ion concentrations on the cathode surface. The interplay of theory and experiments validates the mechanism, and guides us to functionalize the surface of a Cu cathode with a hydronium-repelling layer to further the pressure-mediated selectivity effect. This work illustrates the value of industrial CO2 sources as the starting feedstock for sustainable chemical synthesis.

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“…When confined by hydrophobic surfaces, a higher solubility is expected due to the coadsorption of CO 2 molecules, whereas a lower solubility is expected for the hydrophilic ones, because of the weak CO 2 −H 2 O interactions. 262,263 Diffusion is also affected by confinement. Overall, CO 2 diffusivity is expected to decrease because the mobility of molecules is reduced; preferential adsorption and steric hindrance may further decrease diffusion.…”

Section: Aqueous Co 2 Diffusion In Confined Mediamentioning

confidence: 99%

Diffusivity of CO₂ in H₂O: A Review of Experimental Studies and Molecular Simulations in the Bulk and in Confinement

Polat,

Coelho,

Vlugt

et al. 2024

J. Chem. Eng. Data

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CO₂ Solubility in Aqueous Electrolyte Solutions Confined in Calcite Nanopores

Cited by 12 publications

References 59 publications

Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Pressure dependence in aqueous-based electrochemical CO2 reduction

Diffusivity of CO₂ in H₂O: A Review of Experimental Studies and Molecular Simulations in the Bulk and in Confinement

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CO2 Solubility in Aqueous Electrolyte Solutions Confined in Calcite Nanopores

Cited by 12 publications

References 59 publications

Fundamental Insight into Humid CO2 Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Fundamental Insight into Humid CO2 Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Pressure dependence in aqueous-based electrochemical CO2 reduction

Diffusivity of CO2 in H2O: A Review of Experimental Studies and Molecular Simulations in the Bulk and in Confinement

Contact Info

Product

Resources

About

CO₂ Solubility in Aqueous Electrolyte Solutions Confined in Calcite Nanopores

Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Fundamental Insight into Humid CO₂ Uptake in Direct Air Capture Nanocomposites Using Fluorescence and Portable NMR Relaxometry

Diffusivity of CO₂ in H₂O: A Review of Experimental Studies and Molecular Simulations in the Bulk and in Confinement