TY - JOUR
T1 - Directed Hydrogen Bond Placement
T2 - Low Viscosity Amine Solvents for CO2 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
N1 - Funding Information:
The authors would like to acknowledge the Department of Energy (DOE), Fossil Energy, Office of Coal for funding this project. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the U.S. Department of Energy under contract DE-AC05-76RL01830. Computer resources were provided by the National Energy Research Center (NERSC) and the PNNL’s Research Computing facility.
PY - 2019/4/15
Y1 - 2019/4/15
N2 - 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. Here, 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.
AB - 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. Here, 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.
KW - Acid-base equilibrium
KW - Amino-pyridines
KW - CO capture
KW - Molecular simulations
KW - Water-lean
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U2 - 10.1021/acssuschemeng.8b05481
DO - 10.1021/acssuschemeng.8b05481
M3 - Article
AN - SCOPUS:85064526967
VL - 7
SP - 7535
EP - 7542
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 8
ER -