Mesoscopic Structure Facilitates Rapid CO2 Transport and Reactivity in CO2 Capture Solvents

Xiao Ying Yu, Juan Yao, David B. Lao, David J. Heldebrant, Zihua Zhu, Deepika Malhotra, Manh Thuong Nguyen, Vassiliki Alexandra Glezakou, Roger Rousseau

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Mass transfer coefficients of CO2 are anomalously high in water-lean solvents as compared to aqueous amines. Such phenomena are intrinsic to the molecular and nanoscale structure of concentrated organic CO2 capture solvents. To decipher the connections, we performed in situ liquid time-of-flight secondary ionization mass spectroscopy on a representative water-lean solvent, 1-((1,3-Dimethylimidazolidin-2-ylidene)amino)propan-2-ol (IPADM-2-BOL). Two-dimensional (2D) and three-dimensional (3D) chemical mapping of the solvent revealed that IPADM-2-BOL exhibited a heterogeneous molecular structure with regions of CO2-free solvent coexisting with clusters of zwitterionic carbonate ions. Chemical mapping were consistent with molecular dynamic simulation results, indicating CO2 diffusing through pockets and channels of unreacted solvent. The observed mesoscopic structure promotes and enhances the diffusion and reactivity of CO2, likely prevalent in other water-lean solvents. This finding suggests that if the size, shape and orientation of the domains can be controlled, more efficient CO2 capture solvents could be developed to enhance mass-transfer and uptake kinetics.

Original languageEnglish
Pages (from-to)5765-5771
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume9
Issue number19
DOIs
Publication statusPublished - Oct 4 2018

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reactivity
mass transfer
Water
molecular structure
Mass transfer
water
Carbonates
Molecular structure
Ionization
Amines
Molecular dynamics
carbonates
amines
mass spectroscopy
Spectroscopy
Ions
molecular dynamics
ionization
Kinetics
Computer simulation

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Mesoscopic Structure Facilitates Rapid CO2 Transport and Reactivity in CO2 Capture Solvents. / Yu, Xiao Ying; Yao, Juan; Lao, David B.; Heldebrant, David J.; Zhu, Zihua; Malhotra, Deepika; Nguyen, Manh Thuong; Glezakou, Vassiliki Alexandra; Rousseau, Roger.

In: Journal of Physical Chemistry Letters, Vol. 9, No. 19, 04.10.2018, p. 5765-5771.

Research output: Contribution to journalArticle

Yu, XY, Yao, J, Lao, DB, Heldebrant, DJ, Zhu, Z, Malhotra, D, Nguyen, MT, Glezakou, VA & Rousseau, R 2018, 'Mesoscopic Structure Facilitates Rapid CO2 Transport and Reactivity in CO2 Capture Solvents', Journal of Physical Chemistry Letters, vol. 9, no. 19, pp. 5765-5771. https://doi.org/10.1021/acs.jpclett.8b02231
Yu, Xiao Ying ; Yao, Juan ; Lao, David B. ; Heldebrant, David J. ; Zhu, Zihua ; Malhotra, Deepika ; Nguyen, Manh Thuong ; Glezakou, Vassiliki Alexandra ; Rousseau, Roger. / Mesoscopic Structure Facilitates Rapid CO2 Transport and Reactivity in CO2 Capture Solvents. In: Journal of Physical Chemistry Letters. 2018 ; Vol. 9, No. 19. pp. 5765-5771.
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