Abstract
Capture of CO 2 from power generation is required for its conversion or sequestration. Toward this goal, numerous CO 2 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 CO 2 -rich loadings. Here, we extend these principles to a new class of pyridine-based molecules with a secondary amine functionality for binding CO 2 . The result is a class of water-lean amines that retains high gravimetric capacity (20%) while exhibiting the lowest CO 2 -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 CO 2 with only a 20 °C temperature swing.
| Original language | English |
|---|---|
| Pages (from-to) | 7535-7542 |
| Number of pages | 8 |
| Journal | ACS Sustainable Chemistry and Engineering |
| Volume | 7 |
| Issue number | 8 |
| DOIs | |
| Publication status | Published - Apr 15 2019 |
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Keywords
- Acid-base equilibrium
- Amino-pyridines
- CO capture
- Molecular simulations
- Water-lean
ASJC Scopus subject areas
- Chemistry(all)
- Environmental Chemistry
- Chemical Engineering(all)
- Renewable Energy, Sustainability and the Environment
Cite this
Directed Hydrogen Bond Placement : Low Viscosity Amine Solvents for CO 2 Capture. / Malhotra, Deepika; Cantu, David C.; Koech, Phillip K.; Heldebrant, David J.; Karkamkar, Abhijeet; Zheng, Feng; Bearden, Mark D.; Rousseau, Roger; Glezakou, Vassiliki Alexandra.
In: ACS Sustainable Chemistry and Engineering, Vol. 7, No. 8, 15.04.2019, p. 7535-7542.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Directed Hydrogen Bond Placement
T2 - Low Viscosity Amine Solvents for CO 2 Capture
AU - Malhotra, Deepika
AU - Cantu, David C.
AU - Koech, Phillip K.
AU - Heldebrant, David J.
AU - Karkamkar, Abhijeet
AU - Zheng, Feng
AU - Bearden, Mark D.
AU - Rousseau, Roger
AU - Glezakou, Vassiliki Alexandra
PY - 2019/4/15
Y1 - 2019/4/15
N2 - Capture of CO 2 from power generation is required for its conversion or sequestration. Toward this goal, numerous CO 2 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 CO 2 -rich loadings. Here, we extend these principles to a new class of pyridine-based molecules with a secondary amine functionality for binding CO 2 . The result is a class of water-lean amines that retains high gravimetric capacity (20%) while exhibiting the lowest CO 2 -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 CO 2 with only a 20 °C temperature swing.
AB - Capture of CO 2 from power generation is required for its conversion or sequestration. Toward this goal, numerous CO 2 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 CO 2 -rich loadings. Here, we extend these principles to a new class of pyridine-based molecules with a secondary amine functionality for binding CO 2 . The result is a class of water-lean amines that retains high gravimetric capacity (20%) while exhibiting the lowest CO 2 -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 CO 2 with only a 20 °C temperature swing.
KW - Acid-base equilibrium
KW - Amino-pyridines
KW - CO capture
KW - Molecular simulations
KW - Water-lean
UR - http://www.scopus.com/inward/record.url?scp=85064526967&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85064526967&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.8b05481
DO - 10.1021/acssuschemeng.8b05481
M3 - Article
VL - 7
SP - 7535
EP - 7542
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 8
ER -