Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation

Handle URI:
http://hdl.handle.net/10754/562662
Title:
Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation
Authors:
Nugent, Patrick S.; Belmabkhout, Youssef ( 0000-0001-9952-5007 ) ; Burd, Stephen D.; Cairns, Amy; Luebke, Ryan ( 0000-0002-1285-3321 ) ; Forrest, Katherine A.; Pham, Tony T.; Ma, Shengqian; Space, Brian; Wojtas, Łukasz; Eddaoudi, Mohamed ( 0000-0003-1916-9837 ) ; Zaworotko, Michael J.
Abstract:
The energy costs associated with the separation and purification of industrial commodities, such as gases, fine chemicals and fresh water, currently represent around 15 per cent of global energy production, and the demand for such commodities is projected to triple by 2050 (ref. 1). The challenge of developing effective separation and purification technologies that have much smaller energy footprints is greater for carbon dioxide (CO2) than for other gases; in addition to its involvement in climate change, CO 2 is an impurity in natural gas, biogas (natural gas produced from biomass), syngas (CO/H 2, the main source of hydrogen in refineries) and many other gas streams. In the context of porous crystalline materials that can exploit both equilibrium and kinetic selectivity, size selectivity and targeted molecular recognition are attractive characteristics for CO 2 separation and capture, as exemplified by zeolites 5A and 13X (ref. 2), as well as metal-organic materials (MOMs). Here we report that a crystal engineering or reticular chemistry strategy that controls pore functionality and size in a series of MOMs with coordinately saturated metal centres and periodically arrayed hexafluorosilicate (SiF 6 2-) anions enables a 'sweet spot' of kinetics and thermodynamics that offers high volumetric uptake at low CO2 partial pressure (less than 0.15 bar). Most importantly, such MOMs offer an unprecedented CO 2 sorption selectivity over N2, H 2 and CH 4, even in the presence of moisture. These MOMs are therefore relevant to CO2 separation in the context of post-combustion (flue gas, CO2/N2), pre-combustion (shifted synthesis gas stream, CO 2/H 2) and natural gas upgrading (natural gas clean-up, CO2/CH 4). © 2013 Macmillan Publishers Limited. All rights reserved.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Functional Materials Design, Discovery and Development (FMD3)
Publisher:
Nature Publishing Group
Journal:
Nature
Issue Date:
27-Feb-2013
DOI:
10.1038/nature11893
PubMed ID:
23446349
Type:
Article
ISSN:
00280836
Sponsors:
This publication is based on work supported by KAUST award number FIC/2010/06 (ME. and M.J.Z.) and KAUST start up funds (RE.). B.S. acknowledges computational resources made available by an XSEDE grant (number TG-DMR090028). Single-crystal diffraction experiments on SIFSIX-2-Cu-I were conducted at the Advanced Photon Source on beamline 15ID-B of ChemMatCARS Sector 15, which is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-0822838. Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract number DE-AC02-06CH11357.
Is Supplemented By:
Nugent, P., Belmabkhout, Y., Burd, S. D., Cairns, A. J., Luebke, R., Forrest, K., … Zaworotko, M. J. (2013). CCDC 914600: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cczpq7l; DOI:10.5517/cczpq7l; HANDLE:http://hdl.handle.net/10754/624765; Nugent, P., Belmabkhout, Y., Burd, S. D., Cairns, A. J., Luebke, R., Forrest, K., … Zaworotko, M. J. (2013). CCDC 914601: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cczpq8m; DOI:10.5517/cczpq8m; HANDLE:http://hdl.handle.net/10754/624766
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorNugent, Patrick S.en
dc.contributor.authorBelmabkhout, Youssefen
dc.contributor.authorBurd, Stephen D.en
dc.contributor.authorCairns, Amyen
dc.contributor.authorLuebke, Ryanen
dc.contributor.authorForrest, Katherine A.en
dc.contributor.authorPham, Tony T.en
dc.contributor.authorMa, Shengqianen
dc.contributor.authorSpace, Brianen
dc.contributor.authorWojtas, Łukaszen
dc.contributor.authorEddaoudi, Mohameden
dc.contributor.authorZaworotko, Michael J.en
dc.date.accessioned2015-08-03T11:00:20Zen
dc.date.available2015-08-03T11:00:20Zen
dc.date.issued2013-02-27en
dc.identifier.issn00280836en
dc.identifier.pmid23446349en
dc.identifier.doi10.1038/nature11893en
dc.identifier.urihttp://hdl.handle.net/10754/562662en
dc.description.abstractThe energy costs associated with the separation and purification of industrial commodities, such as gases, fine chemicals and fresh water, currently represent around 15 per cent of global energy production, and the demand for such commodities is projected to triple by 2050 (ref. 1). The challenge of developing effective separation and purification technologies that have much smaller energy footprints is greater for carbon dioxide (CO2) than for other gases; in addition to its involvement in climate change, CO 2 is an impurity in natural gas, biogas (natural gas produced from biomass), syngas (CO/H 2, the main source of hydrogen in refineries) and many other gas streams. In the context of porous crystalline materials that can exploit both equilibrium and kinetic selectivity, size selectivity and targeted molecular recognition are attractive characteristics for CO 2 separation and capture, as exemplified by zeolites 5A and 13X (ref. 2), as well as metal-organic materials (MOMs). Here we report that a crystal engineering or reticular chemistry strategy that controls pore functionality and size in a series of MOMs with coordinately saturated metal centres and periodically arrayed hexafluorosilicate (SiF 6 2-) anions enables a 'sweet spot' of kinetics and thermodynamics that offers high volumetric uptake at low CO2 partial pressure (less than 0.15 bar). Most importantly, such MOMs offer an unprecedented CO 2 sorption selectivity over N2, H 2 and CH 4, even in the presence of moisture. These MOMs are therefore relevant to CO2 separation in the context of post-combustion (flue gas, CO2/N2), pre-combustion (shifted synthesis gas stream, CO 2/H 2) and natural gas upgrading (natural gas clean-up, CO2/CH 4). © 2013 Macmillan Publishers Limited. All rights reserved.en
dc.description.sponsorshipThis publication is based on work supported by KAUST award number FIC/2010/06 (ME. and M.J.Z.) and KAUST start up funds (RE.). B.S. acknowledges computational resources made available by an XSEDE grant (number TG-DMR090028). Single-crystal diffraction experiments on SIFSIX-2-Cu-I were conducted at the Advanced Photon Source on beamline 15ID-B of ChemMatCARS Sector 15, which is principally supported by the National Science Foundation/Department of Energy under grant number NSF/CHE-0822838. Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract number DE-AC02-06CH11357.en
dc.publisherNature Publishing Groupen
dc.titlePorous materials with optimal adsorption thermodynamics and kinetics for CO2 separationen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentFunctional Materials Design, Discovery and Development (FMD3)en
dc.identifier.journalNatureen
dc.contributor.institutionDepartment of Chemistry, University of South Florida, 4202 East Fowler Avenue, Tampa, FL 33620, United Statesen
kaust.authorBelmabkhout, Youssefen
kaust.authorCairns, Amyen
kaust.authorLuebke, Ryanen
kaust.authorEddaoudi, Mohameden
dc.relation.isSupplementedByNugent, P., Belmabkhout, Y., Burd, S. D., Cairns, A. J., Luebke, R., Forrest, K., … Zaworotko, M. J. (2013). CCDC 914600: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cczpq7len
dc.relation.isSupplementedByDOI:10.5517/cczpq7len
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624765en
dc.relation.isSupplementedByNugent, P., Belmabkhout, Y., Burd, S. D., Cairns, A. J., Luebke, R., Forrest, K., … Zaworotko, M. J. (2013). CCDC 914601: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cczpq8men
dc.relation.isSupplementedByDOI:10.5517/cczpq8men
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624766en
All Items in KAUST are protected by copyright, with all rights reserved, unless otherwise indicated.