Directed Hydrogen Bond Placement: Low Viscosity Amine Solvents for CO2 Capture
Abstract
Capture of CO2 from power generation is required for its conversion or sequestration. Toward this goal, numerous CO2 capture processes have been developed, with the most widely deployed technology utilizing aqueous solutions of amines. Our group has focused on the design of several classes of water-lean solvents in order to identify molecular-level descriptors to control materials properties such as viscosity and regeneration energy. Density functional theory calculations and classical molecular dynamic simulations have shown that strategic placement of hydrogen bonding and tuning of the acid/base equilibria are critical for controlling viscosity at CO2-rich loadings. In this work, we extend these principles to a new class of pyridine-based molecules with a secondary amine functionality for binding CO2. The result is a class of water-lean amines that retains high gravimetric capacity (20%) while exhibiting the lowest CO2-rich viscosities (<150 cP, 40 °C) of any 100% concentrated amine currently known. Additionally, these newly identified solvents exhibit regeneration temperatures as low as 60 °C when applying a polarity swing assisted regeneration, resulting in a solvent that can conceptually absorb and desorb CO2 with only a 20 °C temperature swing.
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Nevada, Reno, NV (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1542884
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Sustainable Chemistry & Engineering
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 8; Journal ID: ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; amino-pyridines; CO2 capture; water-lean; acid-base equilibrium; molecular simulations
Citation Formats
Malhotra, Deepika, Cantu, David C., Koech, Phillip K., Heldebrant, David J., Karkamkar, Abhijeet, Zheng, Feng, Bearden, Mark D., Rousseau, Roger, and Glezakou, Vassiliki-Alexandra. Directed Hydrogen Bond Placement: Low Viscosity Amine Solvents for CO2 Capture. United States: N. p., 2019.
Web. doi:10.1021/acssuschemeng.8b05481.
Malhotra, Deepika, Cantu, David C., Koech, Phillip K., Heldebrant, David J., Karkamkar, Abhijeet, Zheng, Feng, Bearden, Mark D., Rousseau, Roger, & Glezakou, Vassiliki-Alexandra. Directed Hydrogen Bond Placement: Low Viscosity Amine Solvents for CO2 Capture. United States. https://doi.org/10.1021/acssuschemeng.8b05481
Malhotra, Deepika, Cantu, David C., Koech, Phillip K., Heldebrant, David J., Karkamkar, Abhijeet, Zheng, Feng, Bearden, Mark D., Rousseau, Roger, and Glezakou, Vassiliki-Alexandra. Fri .
"Directed Hydrogen Bond Placement: Low Viscosity Amine Solvents for CO2 Capture". United States. https://doi.org/10.1021/acssuschemeng.8b05481. https://www.osti.gov/servlets/purl/1542884.
@article{osti_1542884,
title = {Directed Hydrogen Bond Placement: Low Viscosity Amine Solvents for CO2 Capture},
author = {Malhotra, Deepika and Cantu, David C. and Koech, Phillip K. and Heldebrant, David J. and Karkamkar, Abhijeet and Zheng, Feng and Bearden, Mark D. and Rousseau, Roger and Glezakou, Vassiliki-Alexandra},
abstractNote = {Capture of CO2 from power generation is required for its conversion or sequestration. Toward this goal, numerous CO2 capture processes have been developed, with the most widely deployed technology utilizing aqueous solutions of amines. Our group has focused on the design of several classes of water-lean solvents in order to identify molecular-level descriptors to control materials properties such as viscosity and regeneration energy. Density functional theory calculations and classical molecular dynamic simulations have shown that strategic placement of hydrogen bonding and tuning of the acid/base equilibria are critical for controlling viscosity at CO2-rich loadings. In this work, we extend these principles to a new class of pyridine-based molecules with a secondary amine functionality for binding CO2. The result is a class of water-lean amines that retains high gravimetric capacity (20%) while exhibiting the lowest CO2-rich viscosities (<150 cP, 40 °C) of any 100% concentrated amine currently known. Additionally, these newly identified solvents exhibit regeneration temperatures as low as 60 °C when applying a polarity swing assisted regeneration, resulting in a solvent that can conceptually absorb and desorb CO2 with only a 20 °C temperature swing.},
doi = {10.1021/acssuschemeng.8b05481},
journal = {ACS Sustainable Chemistry & Engineering},
number = 8,
volume = 7,
place = {United States},
year = {Fri Mar 15 00:00:00 EDT 2019},
month = {Fri Mar 15 00:00:00 EDT 2019}
}
Web of Science
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