New sterically hindered polyvinylamine-containing membranes for CO2 capture from flue gas

Chen, Ting-Yu; Deng, Xuepeng; Lin, Li-Chiang; Ho, W.S. Winston

doi:10.1016/j.memsci.2021.120195

Title: New sterically hindered polyvinylamine-containing membranes for CO₂ capture from flue gas

Journal Article · Tue Dec 21 00:00:00 EST 2021 · Journal of Membrane Science

DOI:https://doi.org/10.1016/j.memsci.2021.120195· OSTI ID:1841190

Chen, Ting-Yu ^[1];

^[1]; Lin, Li-Chiang ^[2];

^[1]

The Ohio State Univ., Columbus, OH (United States)
The Ohio State Univ., Columbus, OH (United States); National Taiwan Univ., Taipei (Taiwan)

Amine-containing facilitated transport membranes can have both high permeability and selectivity due to the reversible reaction between CO₂ and amino groups for effective carbon capture from flue gas. In this study, we have developed an improved method for the synthesis of high-molecular-weight sterically hindered polyvinylamine (PVAm) as the new fixed-site carrier in thin-film composite membranes for CO₂ capture. Commercially available PVAm was N-monomethylated into poly-N-methyl-N-vinylamine (PVAm-CH₃) using the stepwise reductive amination with a highly polar fluorinated alcohol as the solvent to enhance the equilibrium shift to the formation of the imine intermediate. The method prevented over-alkylation, resulting in the increased yield of the target product. PVAm-CH₃ exhibited excellent CO₂ facilitation with a CO₂ permeability of 445.7 Barrer (1 Barrer = 3.349 x 10^–16 mol m m^–2 s^–1 Pa^–1) and a CO₂/N₂ selectivity of 70.3, which are above the Robeson 2008 upper bound. The PVAm-CH₃ solution retained a sufficiently high viscosity after incorporating the aminoacid salt, 2-(1-piperazinyl)ethylamine sarcosinate (PZEA-Sar), as the mobile carrier for the membrane coating on nanoporous polyethersulfone (PES) substrates without any penetration issues. The resultant thin-film composite PVAm-CH3/PZEA-Sar membrane with a thickness of approximately 170 nm exhibited a superior CO₂ performance of 1071 GPU (1 GPU = 3.349 x 10^–10 mol m^–2 s^–1 Pa^–1) and a CO₂/N₂ selectivity of 183 at 57°C and a feed gas pressure of 111.64 kPa (1.5 psig). This PVAm-CH₃/PZEA-Sar membrane surpassed the latest redefined 2019 CO₂/N₂ upper bound and outperformed other polymer-based membranes. Density functional theory calculations also demonstrated that PVAm-CH₃ showed a stronger preference, relative to PVAm, toward the more efficient bicarbonate pathway. Thus, the steric hindrance effect of PVAm-CH₃ enhanced the solubility of CO₂ in the polymer matrix and resulted in the higher CO₂ permeance.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE; Ohio Development Services Agency

Grant/Contract Number:: FE0031731; OER-CDO-D-19-12

OSTI ID:: 1841190

Alternate ID(s):: OSTI ID: 1837380

Journal Information:: Journal of Membrane Science, Vol. 645; ISSN 0376-7388

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: New sterically hindered polyvinylamine-containing membranes for CO2 capture from flue gas

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Title: New sterically hindered polyvinylamine-containing membranes for CO₂ capture from flue gas