A cooperative adsorbent for the switch-like capture of carbon dioxide from crude natural gas
Natural gas constitutes a growing share of global primary energy due to its abundant supply and lower CO 2 emission intensity compared to coal. For many natural gas reserves, CO 2 contamination must be removed at the wellhead to meet pipeline specifications. Here, we demonstrate the potential of the...
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Published in | Chemical science (Cambridge) Vol. 13; no. 4; pp. 11772 - 11784 |
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Main Authors | , , , , |
Format | Journal Article |
Language | English |
Published |
Cambridge
Royal Society of Chemistry
19.10.2022
Royal Society of Chemistry (RSC) The Royal Society of Chemistry |
Subjects | |
Online Access | Get full text |
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Summary: | Natural gas constitutes a growing share of global primary energy due to its abundant supply and lower CO
2
emission intensity compared to coal. For many natural gas reserves, CO
2
contamination must be removed at the wellhead to meet pipeline specifications. Here, we demonstrate the potential of the diamine-appended metal-organic framework ee-2-Mg
2
(dobpdc) (ee-2 =
N
,
N
-diethylethylenediamine; dobpdc
4−
= 4,4′-dioxidobiphenyl-3,3′-dicarboxylate) as a next-generation CO
2
capture material for high-pressure natural gas purification. Owing to a cooperative adsorption mechanism involving formation of ammonium carbamate chains, ee-2-Mg
2
(dobpdc) can be readily regenerated with a minimal change in temperature or pressure and maintains its CO
2
capacity in the presence of water. Moreover, breakthrough experiments reveal that water enhances the CO
2
capture performance of ee-2-Mg
2
(dobpdc) by eliminating "slip" of CO
2
before full breakthrough. Spectroscopic characterization and multicomponent adsorption isobars suggest that the enhanced performance under humid conditions arises from preferential stabilization of the CO
2
-inserted phase in the presence of water. The favorable performance of ee-2-Mg
2
(dobpdc) is further demonstrated through comparison with a benchmark material for this separation, zeolite 13X, as well as extended pressure cycling. Overall, these results support continued development of ee-2-Mg
2
(dobpdc) as a promising adsorbent for natural gas purification.
Diamine-appended metal-organic frameworks can be optimized as adsorbents for pressure-swing purification of crude natural gas. A cooperative CO
2
binding mechanism enables high CO
2
swing capacities and enhanced performance under humid conditions. |
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Bibliography: | For ESI and crystallographic data in CIF or other electronic format see Electronic supplementary information (ESI) available: Supplementary figures, adsorption isotherms and fits, crystallographic information. CCDC 1912757 https://doi.org/10.1039/d2sc03570g ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 AC02-05CH11231; AC02-06CH11357; SC0001015; SC0019992 USDOE Current address: Harvard University, Cambridge, MA 02138, USA. Current address: Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA. |
ISSN: | 2041-6520 2041-6539 |
DOI: | 10.1039/d2sc03570g |