Chemical Feedback in the Self-Assembly and Function of Air-Liquid Interfaces: Insight into the Bottlenecks of CO2 Direct Air Capture

Uvinduni I. Premadasa; Dengpan Dong; Diana Stamberga; Radu Custelcean; Santanu Roy; Ying Zhong Ma; Vera Bocharova; Vyacheslav S. Bryantsev; Benjamin Doughty

doi:10.1021/acsami.3c00719

Chemical Feedback in the Self-Assembly and Function of Air-Liquid Interfaces: Insight into the Bottlenecks of CO₂ Direct Air Capture

Uvinduni I. Premadasa, Dengpan Dong, Diana Stamberga, Radu Custelcean, Santanu Roy, Ying Zhong Ma, Vera Bocharova, Vyacheslav S. Bryantsev, Benjamin Doughty

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

As fossil fuels remain a major source of energy throughout the world, developing efficient negative emission technologies, such as direct air capture (DAC), which remove carbon dioxide (CO₂) from the air, becomes critical for mitigating climate change. Although all DAC processes involve CO₂ transport from air into a sorbent/solvent, through an air-solid or air-liquid interface, the fundamental roles the interfaces play in DAC remain poorly understood. Herein, we study the interfacial behavior of amino acid (AA) solvents used in DAC through a combination of vibrational sum frequency generation spectroscopy and molecular dynamics simulations. This study revealed that the absorption of atmospheric CO₂ has antagonistic effects on subsequent capture events that are driven by changes in bulk pH and specific ion effects that feedback on surface organization and interactions. Among the three AAs (leucine, valine, and phenylalanine) studied, we identify and separate behaviors from CO₂ loading, chemical changes, variations in pH, and specific ion effects that tune structural and chemical degrees of freedom at the air-aqueous interface. The fundamental mechanistic findings described here are anticipated to enable new approaches to DAC based on exploiting interfaces as a tool to address climate change.

Original language	English
Pages (from-to)	19634-19645
Number of pages	12
Journal	ACS Applied Materials and Interfaces
Volume	15
Issue number	15
DOIs	https://doi.org/10.1021/acsami.3c00719
State	Published - Apr 19 2023

Funding

All authors were supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Separation Sciences. This work was produced by UT-Battelle LLC under contract no. DE-AC05-00OR22725 with the U. S. Department of Energy. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory and in part by the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract no. DE-AC02-05CH11231. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Acknowledgments

Keywords

climate change
non-equilibrium
sorbents
specific ion
vibrational spectroscopy

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1021/acsami.3c00719

Cite this

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title = "Chemical Feedback in the Self-Assembly and Function of Air-Liquid Interfaces: Insight into the Bottlenecks of CO2 Direct Air Capture",

abstract = "As fossil fuels remain a major source of energy throughout the world, developing efficient negative emission technologies, such as direct air capture (DAC), which remove carbon dioxide (CO2) from the air, becomes critical for mitigating climate change. Although all DAC processes involve CO2 transport from air into a sorbent/solvent, through an air-solid or air-liquid interface, the fundamental roles the interfaces play in DAC remain poorly understood. Herein, we study the interfacial behavior of amino acid (AA) solvents used in DAC through a combination of vibrational sum frequency generation spectroscopy and molecular dynamics simulations. This study revealed that the absorption of atmospheric CO2 has antagonistic effects on subsequent capture events that are driven by changes in bulk pH and specific ion effects that feedback on surface organization and interactions. Among the three AAs (leucine, valine, and phenylalanine) studied, we identify and separate behaviors from CO2 loading, chemical changes, variations in pH, and specific ion effects that tune structural and chemical degrees of freedom at the air-aqueous interface. The fundamental mechanistic findings described here are anticipated to enable new approaches to DAC based on exploiting interfaces as a tool to address climate change.",

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N2 - As fossil fuels remain a major source of energy throughout the world, developing efficient negative emission technologies, such as direct air capture (DAC), which remove carbon dioxide (CO2) from the air, becomes critical for mitigating climate change. Although all DAC processes involve CO2 transport from air into a sorbent/solvent, through an air-solid or air-liquid interface, the fundamental roles the interfaces play in DAC remain poorly understood. Herein, we study the interfacial behavior of amino acid (AA) solvents used in DAC through a combination of vibrational sum frequency generation spectroscopy and molecular dynamics simulations. This study revealed that the absorption of atmospheric CO2 has antagonistic effects on subsequent capture events that are driven by changes in bulk pH and specific ion effects that feedback on surface organization and interactions. Among the three AAs (leucine, valine, and phenylalanine) studied, we identify and separate behaviors from CO2 loading, chemical changes, variations in pH, and specific ion effects that tune structural and chemical degrees of freedom at the air-aqueous interface. The fundamental mechanistic findings described here are anticipated to enable new approaches to DAC based on exploiting interfaces as a tool to address climate change.

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