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Hierarchical ion interactions in the direct air capture of CO2 at air/aqueous interfaces.

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Názov: Hierarchical ion interactions in the direct air capture of CO2 at air/aqueous interfaces.
Autori: Premadasa, Uvinduni I., Kumar, Nitesh, Stamberga, Diana, Bocharova, Vera, Damron, Joshua T., Li, Tianyu, Roy, Santanu, Ma, Ying-Zhong, Bryantsev, Vyacheslav S., Doughty, Benjamin
Zdroj: Journal of Chemical Physics; 10/28/2024, Vol. 161 Issue 16, p1-9, 9p
Predmety: PHOTON upconversion, MOLECULAR spectroscopy, MOLECULAR dynamics, MODULATION (Music theory), AMINO acids, CARBONACEOUS aerosols
Abstrakt: The direct air capture (DAC) of CO2 using aqueous solvents is plagued by slow kinetics and interfacial barriers that limit effectiveness in combating climate change. Functionalizing air/aqueous surfaces with charged amphiphiles shows promise in accelerating DAC; however, insight into these interfaces and how they evolve in time remains poorly understood. Specifically, competitive ion interactions between DAC reagents and reaction products feedback onto the interfacial structure, thereby modulating interfacial chemical composition and overall function. In this work, we probe the role of glycine amino acid anions (Gly−), an effective CO2 capture reagent, that promotes the organization of cationic oligomers at air/aqueous interfaces. These surfaces are probed with vibrational sum frequency generation spectroscopy and molecular dynamics simulations. Our findings demonstrate that the competition for surface sites between Gly− and captured carbonaceous anions (HCO3−, CO32−, carbamates) drives changes in surface hydration, which in turn tunes oligomer ordering. This phenomenon is related to a hierarchical ordering of anions at the surface that are electrostatically attracted to the surface and their ability to compete for interfacial water. These results point to new ways to tune interfaces for DAC via stratification of ions based on relative surface propensities and specific ion effects. [ABSTRACT FROM AUTHOR]
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Abstrakt:The direct air capture (DAC) of CO<subscript>2</subscript> using aqueous solvents is plagued by slow kinetics and interfacial barriers that limit effectiveness in combating climate change. Functionalizing air/aqueous surfaces with charged amphiphiles shows promise in accelerating DAC; however, insight into these interfaces and how they evolve in time remains poorly understood. Specifically, competitive ion interactions between DAC reagents and reaction products feedback onto the interfacial structure, thereby modulating interfacial chemical composition and overall function. In this work, we probe the role of glycine amino acid anions (Gly<sup>−</sup>), an effective CO<subscript>2</subscript> capture reagent, that promotes the organization of cationic oligomers at air/aqueous interfaces. These surfaces are probed with vibrational sum frequency generation spectroscopy and molecular dynamics simulations. Our findings demonstrate that the competition for surface sites between Gly<sup>−</sup> and captured carbonaceous anions (HCO<subscript>3</subscript><sup>−</sup>, CO<subscript>3</subscript><sup>2−</sup>, carbamates) drives changes in surface hydration, which in turn tunes oligomer ordering. This phenomenon is related to a hierarchical ordering of anions at the surface that are electrostatically attracted to the surface and their ability to compete for interfacial water. These results point to new ways to tune interfaces for DAC via stratification of ions based on relative surface propensities and specific ion effects. [ABSTRACT FROM AUTHOR]
ISSN:00219606
DOI:10.1063/5.0231272