Molecular-Level Overhaul of γ-Aminopropyl Aminosilicone/Triethylene Glycol Post-Combustion CO2-Capture Solvents

David C. Cantu, Deepika Malhotra, Manh Thuong Nguyen, Phillip K. Koech, Difan Zhang, Vassiliki Alexandra Glezakou, Roger Rousseau, Jordan Page, Richard Zheng, Robert J. Perry, David J. Heldebrant

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

Capturing carbon dioxide from post-combustion gas streams is an energy-intensive process that is required prior to either converting or sequestering CO2. Although a few commercial 1st and 2nd generation aqueous amine technologies have been proposed, the cost of capturing CO2 with these technologies remains high. One approach to decrease costs of capture has been the development of water-lean solvents that aim to increase efficiency by reducing the water content in solution. Water-lean solvents, such as γ-aminopropyl aminosilicone/triethylene glycol (GAP/TEG), are promising technologies, with the potential to halve the parasitic load to a coal-fired power plant, albeit only if high solution viscosities and hydrolysis of the siloxane moieties can be mitigated. This study concerns an integrated multidisciplinary approach to overhaul the GAP/TEG solvent system at the molecular level to mitigate hydrolysis while also reducing viscosity. Cosolvents and diluents are found to have negligible effects on viscosity and are not needed. This finding allows for the design of single-component siloxane-free diamine derivatives with site-specific incorporation of selective chemical moieties for direct placement and orientation of hydrogen bonding to reduce viscosity. Ultimately, these new formulations are less susceptible to hydrolysis and exhibit up to a 98 % reduction in viscosity compared to the initial GAP/TEG formulation.

Original languageEnglish
Pages (from-to)3429-3438
Number of pages10
JournalChemSusChem
Volume13
Issue number13
DOIs
StatePublished - Jul 7 2020
Externally publishedYes

Funding

The authors would like to acknowledge the Department of Energy's Office of Fossil Energy for funding this project under FWP 65872. D.C, V.A.G., and R.R. would like to acknowledge Juntaek Lee for his help in consolidating forcefield parameters. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the US Department of Energy under contract DE-AC05-76RL01830. Computer resources were provided by Research Computing at Pacific Northwest National Laboratory, and the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. The authors would like to acknowledge the Department of Energy's Office of Fossil Energy for funding this project under FWP 65872. D.C, V.A.G., and R.R. would like to acknowledge Juntaek Lee for his help in consolidating forcefield parameters. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the US Department of Energy under contract DE‐AC05‐76RL01830. Computer resources were provided by Research Computing at Pacific Northwest National Laboratory, and the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE‐AC02‐05CH11231.

FundersFunder number
National Energy Research Scientific Computing Center
U.S. Department of Energy Office of ScienceDE-AC02-05CH11231
US Department of EnergyDE-AC05-76RL01830
U.S. Department of EnergyDE‐AC02‐05CH11231, DE‐AC05‐76RL01830
Office of Fossil EnergyFWP 65872
National Energy Research Scientific Computing Center

    Keywords

    • CO capture
    • amines
    • gas purification
    • molecular dynamics
    • solvents

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