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Ultraselective glassy polymer membranes with unprecedented performance for energy-efficient sour gas separation.

ABSTRACT: Membrane-based separation of combined acid gases carbon dioxide and hydrogen sulfide from natural gas streams has attracted increasing academic and commercial interest. These feeds are referred to as "sour," and herein, we report an ultra H2S-selective and exceptionally permeable glassy amidoxime-functionalized polymer of intrinsic microporosity for membrane-based separation. A ternary feed mixture (with 20% H2S:20% CO2:60% CH4) was used to demonstrate that a glassy amidoxime-functionalized membrane provides unprecedented separation performance under challenging feed pressures up to 77 bar. These membranes show extraordinary H2S/CH4 selectivity up to 75 with ultrahigh H2S permeability >4000 Barrers, two to three orders of magnitude higher than commercially available glassy polymeric membranes. We demonstrate that the postsynthesis functionalization of hyper-rigid polymers with appropriate functional polar groups provides a unique design strategy for achieving ultraselective and highly permeable membrane materials for practical natural gas sweetening and additional challenging gas pair separations.

SUBMITTER: Yi S

PROVIDER: S-EPMC6534385 | biostudies-literature | 2019 May

REPOSITORIES: biostudies-literature

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Ultraselective glassy polymer membranes with unprecedented performance for energy-efficient sour gas separation.

Yi Shouliang S Ghanem Bader B Liu Yang Y Pinnau Ingo I Koros William J WJ

Science advances 20190524 5

Membrane-based separation of combined acid gases carbon dioxide and hydrogen sulfide from natural gas streams has attracted increasing academic and commercial interest. These feeds are referred to as "sour," and herein, we report an ultra H2S-selective and exceptionally permeable glassy amidoxime-functionalized polymer of intrinsic microporosity for membrane-based separation. A ternary feed mixture (with 20% H2S:20% CO2:60% CH4) was used to demonstrate ...[more]

PMID: 31139751

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Project description:To prevent greenhouse emissions into the atmosphere, separations like CO2/CH4 and CO2/N2 from natural gas, biogas, and flue gasses are crucial. Polymer membranes gained a key role in gas separations over the past decades, but these polymers are often not organized at a molecular level, which results in a trade-off between permeability and selectivity. In this work, the effect of molecular order and orientation in liquid crystals (LCs) polymer membranes for gas permeation is demonstrated. Using the self-assembly of polymerizable LCs to prepare membranes ensures control over the supramolecular organization and alignment of the building blocks at a molecular level. Robust freestanding LC membranes were fabricated that have various, distinct morphologies (isotropic, nematic cybotactic, and smectic C) and alignment (planar and homeotropic), while using the same chemical composition. Single gas permeation data show that the permeability decreases with increasing molecular order while the ideal gas selectivity of He and CO2 over N2 increases tremendously (36-fold for He/N2 and 21-fold for CO2/N2) when going from randomly ordered to the highly ordered smectic C morphology. The calculated diffusion coefficients showed a 10-fold decrease when going from randomly ordered membranes to ordered smectic C membranes. It is proposed that with increasing molecular order, the free volume elements in the membrane become smaller, which hinders gasses with larger kinetic diameters (Ar, N2) more than gasses with smaller kinetic diameters (He, CO2), inducing selectivity. Comparison of gas sorption and permeation performances of planar and homeotropic aligned smectic C membranes shows the effect of molecular orientation by a 3-fold decrease of the diffusion coefficient of homeotropic aligned smectic C membranes resulting in a diminished gas permeation and increased ideal gas selectivities. These results strongly highlight the importance of molecular order and orientation in LC polymer membranes for gas separation.

Dataset Information

Ultraselective glassy polymer membranes with unprecedented performance for energy-efficient sour gas separation.

Publications

Ultraselective glassy polymer membranes with unprecedented performance for energy-efficient sour gas separation.

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