Dialing in Direct Air Capture of CO2 by Crystal Engineering of Bis-iminoguanidines
Abstract
Direct air capture (DAC) technologies that extract carbon dioxide from the atmosphere via chemical processes have the potential to restore the atmospheric CO2 concentration to an optimal level. This study elucidates structure-property relationships in DAC by crystallization of bis-iminoguanidine (BIG) carbonate salts. Here, their crystal structures are analyzed by X-ray and neutron diffraction to accurately measure key structural parameters including molecular conformations, hydrogen bonding, and π-stacking. Experimental measurements of key properties, such as aqueous solubilities and regeneration energies and temperatures, are complemented by first-principles calculations of lattice and hydration free energies, as well as free energies of reactions with CO2, and BIG regenerations. Minor structural modifications in the molecular structure of the BIGs are found to result in major changes in the crystal structures and the aqueous solubilities within the series, leading to enhanced DAC.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1657966
- Alternate Identifier(s):
- OSTI ID: 1646549
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemSusChem
- Additional Journal Information:
- Journal Volume: TBD; Journal Issue: TBD; Journal ID: ISSN 1864-5631
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; direct air capture; carbon dioxide fixation; guanidines; hydrogen bonds; crystallization
Citation Formats
Custelcean, Radu, Williams, Neil J., Wang, Xiaoping, Garrabrant, Kathleen A., Martin, Halie J., Kidder, Michelle K., Ivanov, Alexander S., and Bryantsev, Vyacheslav S. Dialing in Direct Air Capture of CO2 by Crystal Engineering of Bis-iminoguanidines. United States: N. p., 2020.
Web. doi:10.1002/cssc.202001114.
Custelcean, Radu, Williams, Neil J., Wang, Xiaoping, Garrabrant, Kathleen A., Martin, Halie J., Kidder, Michelle K., Ivanov, Alexander S., & Bryantsev, Vyacheslav S. Dialing in Direct Air Capture of CO2 by Crystal Engineering of Bis-iminoguanidines. United States. https://doi.org/10.1002/cssc.202001114
Custelcean, Radu, Williams, Neil J., Wang, Xiaoping, Garrabrant, Kathleen A., Martin, Halie J., Kidder, Michelle K., Ivanov, Alexander S., and Bryantsev, Vyacheslav S. Mon .
"Dialing in Direct Air Capture of CO2 by Crystal Engineering of Bis-iminoguanidines". United States. https://doi.org/10.1002/cssc.202001114. https://www.osti.gov/servlets/purl/1657966.
@article{osti_1657966,
title = {Dialing in Direct Air Capture of CO2 by Crystal Engineering of Bis-iminoguanidines},
author = {Custelcean, Radu and Williams, Neil J. and Wang, Xiaoping and Garrabrant, Kathleen A. and Martin, Halie J. and Kidder, Michelle K. and Ivanov, Alexander S. and Bryantsev, Vyacheslav S.},
abstractNote = {Direct air capture (DAC) technologies that extract carbon dioxide from the atmosphere via chemical processes have the potential to restore the atmospheric CO2 concentration to an optimal level. This study elucidates structure-property relationships in DAC by crystallization of bis-iminoguanidine (BIG) carbonate salts. Here, their crystal structures are analyzed by X-ray and neutron diffraction to accurately measure key structural parameters including molecular conformations, hydrogen bonding, and π-stacking. Experimental measurements of key properties, such as aqueous solubilities and regeneration energies and temperatures, are complemented by first-principles calculations of lattice and hydration free energies, as well as free energies of reactions with CO2, and BIG regenerations. Minor structural modifications in the molecular structure of the BIGs are found to result in major changes in the crystal structures and the aqueous solubilities within the series, leading to enhanced DAC.},
doi = {10.1002/cssc.202001114},
journal = {ChemSusChem},
number = TBD,
volume = TBD,
place = {United States},
year = {Mon Jul 20 00:00:00 EDT 2020},
month = {Mon Jul 20 00:00:00 EDT 2020}
}
Web of Science
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