Photochemically-Driven CO2 Release Using a Metastable-State Photoacid for Energy Efficient Direct Air Capture

Uvinduni I. Premadasa; Vera Bocharova; Audrey R. Miles; Diana Stamberga; Stella Belony; Vyacheslav S. Bryantsev; Adnan Elgattar; Yi Liao; Joshua T. Damron; Michelle K. Kidder; Benjamin Doughty; Radu Custelcean; Ying Zhong Ma

doi:10.1002/anie.202304957

Photochemically-Driven CO₂ Release Using a Metastable-State Photoacid for Energy Efficient Direct Air Capture

Uvinduni I. Premadasa, Vera Bocharova, Audrey R. Miles, Diana Stamberga, Stella Belony, Vyacheslav S. Bryantsev, Adnan Elgattar, Yi Liao, Joshua T. Damron, Michelle K. Kidder, Benjamin Doughty, Radu Custelcean, Ying Zhong Ma

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

17 Scopus citations

Abstract

One of the grand challenges underlying current direct air capture (DAC) technologies relates to the intensive energy cost for sorbent regeneration and CO₂ release, making the massive scale (GtCO₂/year) deployment required to have a positive impact on climate change economically unfeasible. This challenge underscores the critical need to develop new DAC processes with substantially reduced regeneration energies. Here, we report a photochemically-driven approach for CO₂ release by exploiting the unique properties of an indazole metastable-state photoacid (mPAH). Our measurements on simulated and amino acid-based DAC systems revealed the potential of mPAH to be used for CO₂ release cycles by regulating pH changes and associated isomers driven by light. Upon irradiating with moderate intensity light, a ≈55 % and ≈68 % to ≈78 % conversion of total inorganic carbon to CO₂ was found for the simulated and amino acid-based DAC systems, respectively. Our results confirm the feasibility of on-demand CO₂ release under ambient conditions using light instead of heat, thereby providing an energy efficient pathway for the regeneration of DAC sorbents.

Original language	English
Article number	e202304957
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	29
DOIs	https://doi.org/10.1002/anie.202304957
State	Published - Jul 17 2023

Funding

This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Separation Sciences. M. K. K. was supported under award DE-SC0022214 contract FWP ERKPCG25. A.R.M. and S.B. were supported in part by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS) under the Science Undergraduate Laboratory Internships program. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy 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). This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Separation Sciences. M. K. K. was supported under award DE‐SC0022214 contract FWP ERKPCG25. A.R.M. and S.B. were supported in part by the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS) under the Science Undergraduate Laboratory Internships program. This manuscript has been authored by UT‐Battelle, LLC under Contract No. DE‐AC05‐00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non‐exclusive, paid‐up, irrevocable, world‐wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy 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 ).

Funders	Funder number
DOE Public Access Plan
Office of Workforce Development for Teachers	DE-AC05-00OR22725
Separation Sciences	FWP ERKPCG25
United States Government
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

Amino Acids
CO Release
Carbon Storage
Metastable Compounds
Photochemistry

UN SDGs

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

Access to Document

10.1002/anie.202304957

Cite this

Premadasa, U. I., Bocharova, V., Miles, A. R., Stamberga, D., Belony, S., Bryantsev, V. S., Elgattar, A., Liao, Y., Damron, J. T., Kidder, M. K., Doughty, B., Custelcean, R., & Ma, Y. Z. (2023). Photochemically-Driven CO₂ Release Using a Metastable-State Photoacid for Energy Efficient Direct Air Capture. Angewandte Chemie - International Edition, 62(29), Article e202304957. https://doi.org/10.1002/anie.202304957

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Premadasa, UI , Bocharova, V, Miles, AR, Stamberga, D, Belony, S, Bryantsev, VS, Elgattar, A, Liao, Y, Damron, JT, Kidder, MK , Doughty, B , Custelcean, R & Ma, YZ 2023, 'Photochemically-Driven CO₂ Release Using a Metastable-State Photoacid for Energy Efficient Direct Air Capture', Angewandte Chemie - International Edition, vol. 62, no. 29, e202304957. https://doi.org/10.1002/anie.202304957

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AU - Belony, Stella

AU - Bryantsev, Vyacheslav S.

AU - Elgattar, Adnan

AU - Liao, Yi

AU - Damron, Joshua T.

AU - Kidder, Michelle K.

AU - Doughty, Benjamin

AU - Custelcean, Radu

AU - Ma, Ying Zhong

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