Hierarchical Ion Interactions in the Direct Air Capture of CO2 at Air/Aqueous Interfaces

Premadasa, Uvinduni I.; Nln, Nitesh Kumar; Stamberga, Diana; Bocharova, Vera; Damron, Joshua T.; Li, Tianyu; Roy, Santanu; Ma, Ying-zhong; Bryantsev, Vyacheslav S.; Doughty, Benjamin L.

doi:10.1063/5.0231272

Hierarchical Ion Interactions in the Direct Air Capture of CO₂ at Air/Aqueous Interfaces

Journal Article · Fri Oct 25 00:00:00 EDT 2024 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0231272· OSTI ID:2478339

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2478339

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 161; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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