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Title: Mixed-Matric Membranes for CO2 and H2 Gas Separations Using Metal-Organic Framework and Mesoporus Hybrid Silicas

Abstract

In this work, we have investigated the separation performance of polymer-based mixed-matrix membranes containing metal-organic frameworks and mesoporous hybrid silicas. The MOF/Matrimid{reg_sign} and MOP-18/Matrimid{reg_sign} membranes exhibited improved dispersion and mechanical strength that allowed high additive loadings with reduced aggregation, as is the case of the 80 wt% MOP-18/Matrimid{reg_sign} and the 80% (w/w) Cu-MOF/Matrimid{reg_sign} membranes. Membranes with up to 60% (w/w) ZIF-8 content exhibited similar mechanical strength and improved dispersion. The H{sub 2}/CO{sub 2} separation properties of MOF/Matrimid{reg_sign} mixed-matrix membranes was improved by either keeping the selectivity constant and increasing the permeability (MOF-5, Cu-MOF) or by improving both selectivity and permeability (ZIF-8). In the case of MOF-5/Matrimid{reg_sign} mixed-matrix membranes, the H{sub 2}/CO{sub 2} selectivity was kept at 2.6 and the H{sub 2} permeability increased from 24.4 to 53.8 Barrers. For the Cu-MOF/Matrimid{reg_sign} mixed-matrix membranes, the H{sub 2}/CO{sub 2} selectivity was kept at 2.05 and the H{sub 2} permeability increased from 17.1 to 158 Barrers. These two materials introduced porosity and uniform paths that enhanced the gas transport in the membranes. When ZIF-8/Matrimid{reg_sign} mixed-matrix membranes were studied, the H{sub 2}/CO{sub 2} selectivity increased from 2.9 to 4.4 and the permeability of H{sub 2} increased from 26.5 to 35.8 Barrers. The increased H{submore » 2}/CO{sub 2} selectivity in ZIF-8/Matrimid{reg_sign} membranes was explained by the sieving effect introduced by the ZIF-8 crystals (pore window 0.34 nm) that restricted the transport of molecules larger than H{sub 2}. Materials with microporous and/or mesoporous cavities like carbon aerogel composites with zeolite A and zeolite Y, and membranes containing mesoporous ZSM-5 showed sieving effects for small molecules (e.g. H{sub 2} and CO{sub 2}), however, the membranes were most selective for CO{sub 2} due to the strong interaction of the zeolites with CO{sub 2}. For example, at 30 wt% ZSM-5 loading, the CO{sub 2}/CH{sub 4} selectivity increased from 34.7 (Matrimid{reg_sign}) to 56.4. The large increase in selectivity was the result of the increase in CO{sub 2} permeability from 7.3 (Matrimid{reg_sign}) to 14.6 Barrers. At 30 wt% ZSM-5 loading, the H{sub 2}/CH{sub 4} separation was also improved from 83.3 (Matrimid{reg_sign}) to 136.7 with an increase in H{sub 2} permeability from 17.5 (Matrimid{reg_sign}) to 35.3 Barrers. The 10% carbon aerogel-zeolite A and -zeolite Y composite/Matrimid{reg_sign} membranes exhibited an increase in the CO{sub 2}/CH{sub 4} separation from 34.7 to 71.5 (zeolite A composite) and to 57.4 (zeolite Y composite); in addition, the membrane exhibited an increase in the CO{sub 2}/N{sub 2} separation from 33.1 to 50 (zeolite A composite) and to 49.4 (zeolite Y composite), indicating that these type of materials have affinity for CO{sub 2}. The inclusion of mesoporosity enhanced the dispersion of the additive allowing loadings of up to 30% (w/w) without the formation of non-selective voids.« less

Authors:
; ;
Publication Date:
Research Org.:
Univ. of Texas at Dallas, Richardson, TX (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
945031
DOE Contract Number:  
FG26-04NT42173
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; ADDITIVES; AFFINITY; CARBON; CAVITIES; MEMBRANES; PERFORMANCE; PERMEABILITY; POROSITY; STRONG INTERACTIONS; TRANSPORT; ZEOLITES

Citation Formats

Musselman, Inga, Balkus, Jr, Kenneth, and Ferraris, John. Mixed-Matric Membranes for CO2 and H2 Gas Separations Using Metal-Organic Framework and Mesoporus Hybrid Silicas. United States: N. p., 2009. Web. doi:10.2172/945031.
Musselman, Inga, Balkus, Jr, Kenneth, & Ferraris, John. Mixed-Matric Membranes for CO2 and H2 Gas Separations Using Metal-Organic Framework and Mesoporus Hybrid Silicas. United States. doi:10.2172/945031.
Musselman, Inga, Balkus, Jr, Kenneth, and Ferraris, John. Wed . "Mixed-Matric Membranes for CO2 and H2 Gas Separations Using Metal-Organic Framework and Mesoporus Hybrid Silicas". United States. doi:10.2172/945031. https://www.osti.gov/servlets/purl/945031.
@article{osti_945031,
title = {Mixed-Matric Membranes for CO2 and H2 Gas Separations Using Metal-Organic Framework and Mesoporus Hybrid Silicas},
author = {Musselman, Inga and Balkus, Jr, Kenneth and Ferraris, John},
abstractNote = {In this work, we have investigated the separation performance of polymer-based mixed-matrix membranes containing metal-organic frameworks and mesoporous hybrid silicas. The MOF/Matrimid{reg_sign} and MOP-18/Matrimid{reg_sign} membranes exhibited improved dispersion and mechanical strength that allowed high additive loadings with reduced aggregation, as is the case of the 80 wt% MOP-18/Matrimid{reg_sign} and the 80% (w/w) Cu-MOF/Matrimid{reg_sign} membranes. Membranes with up to 60% (w/w) ZIF-8 content exhibited similar mechanical strength and improved dispersion. The H{sub 2}/CO{sub 2} separation properties of MOF/Matrimid{reg_sign} mixed-matrix membranes was improved by either keeping the selectivity constant and increasing the permeability (MOF-5, Cu-MOF) or by improving both selectivity and permeability (ZIF-8). In the case of MOF-5/Matrimid{reg_sign} mixed-matrix membranes, the H{sub 2}/CO{sub 2} selectivity was kept at 2.6 and the H{sub 2} permeability increased from 24.4 to 53.8 Barrers. For the Cu-MOF/Matrimid{reg_sign} mixed-matrix membranes, the H{sub 2}/CO{sub 2} selectivity was kept at 2.05 and the H{sub 2} permeability increased from 17.1 to 158 Barrers. These two materials introduced porosity and uniform paths that enhanced the gas transport in the membranes. When ZIF-8/Matrimid{reg_sign} mixed-matrix membranes were studied, the H{sub 2}/CO{sub 2} selectivity increased from 2.9 to 4.4 and the permeability of H{sub 2} increased from 26.5 to 35.8 Barrers. The increased H{sub 2}/CO{sub 2} selectivity in ZIF-8/Matrimid{reg_sign} membranes was explained by the sieving effect introduced by the ZIF-8 crystals (pore window 0.34 nm) that restricted the transport of molecules larger than H{sub 2}. Materials with microporous and/or mesoporous cavities like carbon aerogel composites with zeolite A and zeolite Y, and membranes containing mesoporous ZSM-5 showed sieving effects for small molecules (e.g. H{sub 2} and CO{sub 2}), however, the membranes were most selective for CO{sub 2} due to the strong interaction of the zeolites with CO{sub 2}. For example, at 30 wt% ZSM-5 loading, the CO{sub 2}/CH{sub 4} selectivity increased from 34.7 (Matrimid{reg_sign}) to 56.4. The large increase in selectivity was the result of the increase in CO{sub 2} permeability from 7.3 (Matrimid{reg_sign}) to 14.6 Barrers. At 30 wt% ZSM-5 loading, the H{sub 2}/CH{sub 4} separation was also improved from 83.3 (Matrimid{reg_sign}) to 136.7 with an increase in H{sub 2} permeability from 17.5 (Matrimid{reg_sign}) to 35.3 Barrers. The 10% carbon aerogel-zeolite A and -zeolite Y composite/Matrimid{reg_sign} membranes exhibited an increase in the CO{sub 2}/CH{sub 4} separation from 34.7 to 71.5 (zeolite A composite) and to 57.4 (zeolite Y composite); in addition, the membrane exhibited an increase in the CO{sub 2}/N{sub 2} separation from 33.1 to 50 (zeolite A composite) and to 49.4 (zeolite Y composite), indicating that these type of materials have affinity for CO{sub 2}. The inclusion of mesoporosity enhanced the dispersion of the additive allowing loadings of up to 30% (w/w) without the formation of non-selective voids.},
doi = {10.2172/945031},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2009},
month = {1}
}