Data-driven design of metal–organic frameworks for wet flue gas CO2 capture

Limiting the increase of CO 2 in the atmosphere is one of the largest challenges of our generation 1 . Because carbon capture and storage is one of the few viable technologies that can mitigate current CO 2 emissions 2 , much effort is focused on developing solid adsorbents that can efficiently capt...

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Veröffentlicht in:	Nature (London) Jg. 576; H. 7786; S. 253 - 256
Hauptverfasser:	Boyd, Peter G., Chidambaram, Arunraj, García-Díez, Enrique, Ireland, Christopher P., Daff, Thomas D., Bounds, Richard, Gładysiak, Andrzej, Schouwink, Pascal, Moosavi, Seyed Mohamad, Maroto-Valer, M. Mercedes, Reimer, Jeffrey A., Navarro, Jorge A. R., Woo, Tom K., Garcia, Susana, Stylianou, Kyriakos C., Smit, Berend
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	London Nature Publishing Group UK 12.12.2019 Nature Publishing Group
Schlagworte:	119/118 639/301/1034/1035 639/301/299/921 639/638/630 Adsorption Anthropogenic factors Binding sites Carbon Carbon dioxide Carbon dioxide atmospheric concentrations Carbon dioxide emissions Carbon sequestration Carbon sources Chemical industry Computer applications Data mining Flue gas Gases Humanities and Social Sciences Humidity Hydrogen Hydrophobicity INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Libraries Ligands Materials selection Metal ions Metal-organic frameworks multidisciplinary NMR Nuclear magnetic resonance Organic chemistry Science Science (multidisciplinary) Selectivity Separation
ISSN:	0028-0836, 1476-4687, 1476-4687
Online-Zugang:	Volltext
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Abstract	Limiting the increase of CO 2 in the atmosphere is one of the largest challenges of our generation 1 . Because carbon capture and storage is one of the few viable technologies that can mitigate current CO 2 emissions 2 , much effort is focused on developing solid adsorbents that can efficiently capture CO 2 from flue gases emitted from anthropogenic sources 3 . One class of materials that has attracted considerable interest in this context is metal–organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO 2 from nitrogen 4 – 7 do not perform well when using realistic flue gas that contains water, because water competes with CO 2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive 8 , 9 . Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO 2 -binding sites—which we term ‘adsorbaphores’—that endow MOFs with CO 2 /N 2 selectivity that persists in wet flue gases. We subsequently synthesized two water-stable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process—including the targeted CO 2 sink, such as geological storage or serving as a carbon source for the chemical industry—will be necessary to identify the optimal separation material. Data mining of a computational library of metal–organic frameworks identifies motifs that bind CO 2 sufficiently strongly and whose uptake is not affected by water, with application for the capture of CO 2 from flue gases.
AbstractList	Limiting the increase of CO2 in the atmosphere is one ofthe largest challenges of our generation1. Because carbon capture and storage is one of the few viable technologies that can mitigate current CO2 emissions2, much effort is focused on developing solid adsorbents that can efficiently capture CO2 from flue gases emitted from anthropogenic sources3. One class of materials that has attracted considerable interest in this context is metal-organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO2 from nitrogen4-7 do not perform well when using realistic flue gas that contains water, because water competes with CO2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive8,9. Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO2binding sites-which we term 'adsorbaphores'-that endow MOFs with CO2/N2 selectivity that persists in wet flue gases. We subsequently synthesized two waterstable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process-including the targeted CO2 sink, such as geological storage or serving as a carbon source for the chemical industry-will be necessary to identify the optimal separation material. Limiting the increase of CO2 in the atmosphere is one of the largest challenges of our generation1. Because carbon capture and storage is one of the few viable technologies that can mitigate current CO2 emissions2, much effort is focused on developing solid adsorbents that can efficiently capture CO2 from flue gases emitted from anthropogenic sources3. One class of materials that has attracted considerable interest in this context is metal-organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO2 from nitrogen4-7 do not perform well when using realistic flue gas that contains water, because water competes with CO2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive8,9. Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO2-binding sites-which we term 'adsorbaphores'-that endow MOFs with CO2/N2 selectivity that persists in wet flue gases. We subsequently synthesized two water-stable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process-including the targeted CO2 sink, such as geological storage or serving as a carbon source for the chemical industry-will be necessary to identify the optimal separation material.Limiting the increase of CO2 in the atmosphere is one of the largest challenges of our generation1. Because carbon capture and storage is one of the few viable technologies that can mitigate current CO2 emissions2, much effort is focused on developing solid adsorbents that can efficiently capture CO2 from flue gases emitted from anthropogenic sources3. One class of materials that has attracted considerable interest in this context is metal-organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO2 from nitrogen4-7 do not perform well when using realistic flue gas that contains water, because water competes with CO2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive8,9. Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO2-binding sites-which we term 'adsorbaphores'-that endow MOFs with CO2/N2 selectivity that persists in wet flue gases. We subsequently synthesized two water-stable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process-including the targeted CO2 sink, such as geological storage or serving as a carbon source for the chemical industry-will be necessary to identify the optimal separation material. Limiting the increase of CO2 in the atmosphere is one of the largest challenges of our generation. Because carbon capture and storage is one of the few viable technologies that can mitigate current CO2 emissions, much effort is focused on developing solid adsorbents that can efficiently capture CO2 from flue gases emitted from anthropogenic sources. One class of materials that has attracted considerable interest in this context is metal-organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO2 from nitrogen do not perform well when using realistic flue gas that contains water, because water competes with CO2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive. Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO2-binding sites-which we term 'adsorbaphores'-that endow MOFs with CO2/N2 selectivity that persists in wet flue gases. We subsequently synthesized two water-stable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process-including the targeted CO2 sink, such as geological storage or serving as a carbon source for the chemical industry-will be necessary to identify the optimal separation material. Limiting the increase of CO 2 in the atmosphere is one of the largest challenges of our generation 1 . Because carbon capture and storage is one of the few viable technologies that can mitigate current CO 2 emissions 2 , much effort is focused on developing solid adsorbents that can efficiently capture CO 2 from flue gases emitted from anthropogenic sources 3 . One class of materials that has attracted considerable interest in this context is metal–organic frameworks (MOFs), in which the careful combination of organic ligands with metal-ion nodes can, in principle, give rise to innumerable structurally and chemically distinct nanoporous MOFs. However, many MOFs that are optimized for the separation of CO 2 from nitrogen 4 – 7 do not perform well when using realistic flue gas that contains water, because water competes with CO 2 for the same adsorption sites and thereby causes the materials to lose their selectivity. Although flue gases can be dried, this renders the capture process prohibitively expensive 8 , 9 . Here we show that data mining of a computational screening library of over 300,000 MOFs can identify different classes of strong CO 2 -binding sites—which we term ‘adsorbaphores’—that endow MOFs with CO 2 /N 2 selectivity that persists in wet flue gases. We subsequently synthesized two water-stable MOFs containing the most hydrophobic adsorbaphore, and found that their carbon-capture performance is not affected by water and outperforms that of some commercial materials. Testing the performance of these MOFs in an industrial setting and consideration of the full capture process—including the targeted CO 2 sink, such as geological storage or serving as a carbon source for the chemical industry—will be necessary to identify the optimal separation material. Data mining of a computational library of metal–organic frameworks identifies motifs that bind CO 2 sufficiently strongly and whose uptake is not affected by water, with application for the capture of CO 2 from flue gases.
Author	Woo, Tom K. García-Díez, Enrique Boyd, Peter G. Stylianou, Kyriakos C. Daff, Thomas D. Schouwink, Pascal Maroto-Valer, M. Mercedes Reimer, Jeffrey A. Bounds, Richard Ireland, Christopher P. Moosavi, Seyed Mohamad Garcia, Susana Navarro, Jorge A. R. Chidambaram, Arunraj Gładysiak, Andrzej Smit, Berend
Author_xml	– sequence: 1 givenname: Peter G. surname: Boyd fullname: Boyd, Peter G. organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 2 givenname: Arunraj surname: Chidambaram fullname: Chidambaram, Arunraj organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 3 givenname: Enrique surname: García-Díez fullname: García-Díez, Enrique organization: Research Centre for Carbon Solutions (RCCS), School of Engineering and Physical Sciences, Heriot-Watt University – sequence: 4 givenname: Christopher P. surname: Ireland fullname: Ireland, Christopher P. organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 5 givenname: Thomas D. surname: Daff fullname: Daff, Thomas D. organization: Department of Chemistry and Biomolecular Science, University of Ottawa, Department of Engineering, University of Cambridge – sequence: 6 givenname: Richard surname: Bounds fullname: Bounds, Richard organization: Department of Chemical and Biomolecular Engineering, University of California, Berkeley – sequence: 7 givenname: Andrzej surname: Gładysiak fullname: Gładysiak, Andrzej organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 8 givenname: Pascal surname: Schouwink fullname: Schouwink, Pascal organization: Institut des Sciences et Ingénierie Chimiques (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 9 givenname: Seyed Mohamad surname: Moosavi fullname: Moosavi, Seyed Mohamad organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL) – sequence: 10 givenname: M. Mercedes surname: Maroto-Valer fullname: Maroto-Valer, M. Mercedes organization: Research Centre for Carbon Solutions (RCCS), School of Engineering and Physical Sciences, Heriot-Watt University – sequence: 11 givenname: Jeffrey A. surname: Reimer fullname: Reimer, Jeffrey A. organization: Department of Chemical and Biomolecular Engineering, University of California, Berkeley, Materials Science Division, Lawrence Berkeley National Laboratory – sequence: 12 givenname: Jorge A. R. surname: Navarro fullname: Navarro, Jorge A. R. organization: Departamento de Química Inorgánica, Universidad de Granada – sequence: 13 givenname: Tom K. surname: Woo fullname: Woo, Tom K. email: twoo@uottawa.ca organization: Department of Chemistry and Biomolecular Science, University of Ottawa – sequence: 14 givenname: Susana surname: Garcia fullname: Garcia, Susana email: S.Garcia@hw.ac.uk organization: Research Centre for Carbon Solutions (RCCS), School of Engineering and Physical Sciences, Heriot-Watt University – sequence: 15 givenname: Kyriakos C. surname: Stylianou fullname: Stylianou, Kyriakos C. email: kyriakos.stylianou@oregonstate.edu organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), Department of Chemistry, Oregon State University – sequence: 16 givenname: Berend surname: Smit fullname: Smit, Berend email: berend.smit@epfl.ch organization: Laboratory of Molecular Simulation (LSMO), Institut des Sciences et Ingénierie Chimiques, Valais (ISIC), École Polytechnique Fédérale de Lausanne (EPFL)
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ContentType	Journal Article
Copyright	The Author(s), under exclusive licence to Springer Nature Limited 2019 Copyright Nature Publishing Group Dec 12, 2019
Copyright_xml	– notice: The Author(s), under exclusive licence to Springer Nature Limited 2019 – notice: Copyright Nature Publishing Group Dec 12, 2019
CorporateAuthor	Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States) Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
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References	CouckSAn amine-functionalized MIL-53 metal–organic framework with large separation power for CO2 and CH4J. Am. Chem. Soc.2009131632663271:CAS:528:DC%2BD1MXkslCru7c%3D10.1021/ja900555r GarcíaSBreakthrough adsorption study of a commercial activated carbon for pre-combustion CO2 captureChem. Eng. J.201117154955610.1016/j.cej.2011.04.027 LiGCapture of CO2 from high humidity flue gas by vacuum swing adsorption with zeolite 13XAdsorption2008144154221:CAS:528:DC%2BD1cXjsFajs7s%3D10.1007/s10450-007-9100-y BuiMCarbon capture and storage (CCS): the way forwardEnergy Environ. Sci.201811106211761:CAS:528:DC%2BC1cXls12rurk%3D10.1039/C7EE02342A CarringtonEJVitórica-YrezábalIJBrammerLCrystallographic studies of gas sorption in metal–organic frameworksActa Crystallogr. B2014704044221:CAS:528:DC%2BC2cXpt1Squro%3D10.1107/S2052520614009834 MilnerPJA diaminopropane-appended metal–organic framework enabling efficient CO2 capture from coal flue gas via a mixed adsorption mechanismJ. Am. Chem. 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Soc.200913118198181991:CAS:528:DC%2BD1MXhsFShsr7L10.1021/ja9057234 S Couck (1798_CR13) 2009; 131 TM McDonald (1798_CR11) 2015; 519 N Chanut (1798_CR14) 2017; 10 K Sumida (1798_CR4) 2012; 112 T Loiseau (1798_CR20) 2004; 10 M Bui (1798_CR2) 2018; 11 G Sliwoski (1798_CR16) 2013; 66 A Fateeva (1798_CR19) 2012; 51 H Furukawa (1798_CR5) 2013; 341 S García (1798_CR24) 2011; 171 DM D’Alessandro (1798_CR3) 2010; 49 EJ Carrington (1798_CR23) 2014; 70 JM Huck (1798_CR6) 2014; 7 PG Boyd (1798_CR28) 2017; 2 L-C Lin (1798_CR26) 2012; 11 G Wolber (1798_CR15) 2008; 13 J Merel (1798_CR9) 2008; 47 PJ Milner (1798_CR10) 2017; 139 H Reinsch (1798_CR21) 2013; 171 PG Boyd (1798_CR22) 2016; 18 AO Yazaydin (1798_CR29) 2009; 131 G Li (1798_CR8) 2008; 14 S García (1798_CR25) 2013; 12 CE Wilmer (1798_CR27) 2012; 4 RW Flaig (1798_CR12) 2017; 139 JA Mason (1798_CR7) 2011; 4 KC Stylianou (1798_CR18) 2010; 132 1798_CR1 MT Ho (1798_CR17) 2008; 47
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Snippet	Limiting the increase of CO 2 in the atmosphere is one of the largest challenges of our generation 1 . Because carbon capture and storage is one of the few... Limiting the increase of CO2 in the atmosphere is one ofthe largest challenges of our generation1. Because carbon capture and storage is one of the few viable... Limiting the increase of CO2 in the atmosphere is one of the largest challenges of our generation1. Because carbon capture and storage is one of the few viable... Limiting the increase of CO2 in the atmosphere is one of the largest challenges of our generation. Because carbon capture and storage is one of the few viable...
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SubjectTerms	119/118 639/301/1034/1035 639/301/299/921 639/638/630 Adsorption Anthropogenic factors Binding sites Carbon Carbon dioxide Carbon dioxide atmospheric concentrations Carbon dioxide emissions Carbon sequestration Carbon sources Chemical industry Computer applications Data mining Flue gas Gases Humanities and Social Sciences Humidity Hydrogen Hydrophobicity INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Libraries Ligands Materials selection Metal ions Metal-organic frameworks multidisciplinary NMR Nuclear magnetic resonance Organic chemistry Science Science (multidisciplinary) Selectivity Separation
Title	Data-driven design of metal–organic frameworks for wet flue gas CO2 capture
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