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

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. Data mining of a computational library of metal–organic frameworks identifies motifs that bind CO2 sufficiently strongly and whose uptake is not affected by water, with application for the capture of CO2 from flue gases.

[1]  N. Stock,et al.  High-throughput studies of highly porous Al-based MOFs , 2013 .

[2]  Jeffrey A. Reimer,et al.  Cooperative insertion of CO2 in diamine-appended metal-organic frameworks , 2015, Nature.

[3]  Jun Zhang,et al.  Capture of CO2 from high humidity flue gas by vacuum swing adsorption with zeolite 13X , 2008 .

[4]  S. Chong,et al.  A guest-responsive fluorescent 3D microporous metal-organic framework derived from a long-lifetime pyrene core. , 2010, Journal of the American Chemical Society.

[5]  Li-Chiang Lin,et al.  Evaluating different classes of porous materials for carbon capture , 2014 .

[6]  Thierry Langer,et al.  Molecule-pharmacophore superpositioning and pattern matching in computational drug design. , 2008, Drug discovery today.

[7]  Edward W. Lowe,et al.  Computational Methods in Drug Discovery , 2014, Pharmacological Reviews.

[8]  B. Smit,et al.  Carbon dioxide capture: prospects for new materials. , 2010, Angewandte Chemie.

[9]  Kenji Sumida,et al.  Evaluating metal–organic frameworks for post-combustion carbon dioxide capture via temperature swing adsorption , 2011 .

[10]  Peter G. Boyd,et al.  A generalized method for constructing hypothetical nanoporous materials of any net topology from graph theory , 2016 .

[11]  C. Serre,et al.  Screening the Effect of Water Vapour on Gas Adsorption Performance: Application to CO2 Capture from Flue Gas in Metal-Organic Frameworks. , 2017, ChemSusChem.

[12]  Alexander C. Forse,et al.  A Diaminopropane-Appended Metal-Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism. , 2017, Journal of the American Chemical Society.

[13]  F. Fathieh,et al.  The Chemistry of CO2 Capture in an Amine-Functionalized Metal-Organic Framework under Dry and Humid Conditions. , 2017, Journal of the American Chemical Society.

[14]  M. V. Gil,et al.  Cyclic operation of a fixed-bed pressure and temperature swing process for CO2 capture: Experimental and statistical analysis , 2013 .

[15]  Dianne E. Wiley,et al.  Reducing the Cost of CO2 Capture from Flue Gases Using Pressure Swing Adsorption , 2008 .

[16]  P. Wiper,et al.  A water-stable porphyrin-based metal-organic framework active for visible-light photocatalysis. , 2012, Angewandte Chemie.

[17]  Gérard Férey,et al.  A rationale for the large breathing of the porous aluminum terephthalate (MIL-53) upon hydration. , 2004, Chemistry.

[18]  C. Wilmer,et al.  Large-scale screening of hypothetical metal-organic frameworks. , 2012, Nature chemistry.

[19]  Kenji Sumida,et al.  Carbon dioxide capture in metal-organic frameworks. , 2012, Chemical reviews.

[20]  Peter G. Boyd,et al.  Computational development of the nanoporous materials genome , 2017 .

[21]  Michael O’Keeffe,et al.  The Chemistry and Applications of Metal-Organic Frameworks , 2013, Science.

[22]  M. V. Gil,et al.  Breakthrough adsorption study of a commercial activated carbon for pre-combustion CO2 capture , 2011 .

[23]  L. Brammer,et al.  Crystallographic studies of gas sorption in metal–organic frameworks , 2014, Acta crystallographica Section B, Structural science, crystal engineering and materials.

[24]  Randall Q Snurr,et al.  Screening of metal-organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach. , 2009, Journal of the American Chemical Society.

[25]  Solomon F. Brown,et al.  Carbon capture and storage (CCS): the way forward , 2018 .

[26]  Francis Meunier,et al.  Experimental Investigation on CO2 Post−Combustion Capture by Indirect Thermal Swing Adsorption Using 13X and 5A Zeolites , 2008 .

[27]  Freek Kapteijn,et al.  An amine-functionalized MIL-53 metal-organic framework with large separation power for CO2 and CH4. , 2009, Journal of the American Chemical Society.

[28]  Jeffrey A. Reimer,et al.  INTRODUCTION TO CARBON CAPTURE AND SEQUESTRATION , 2014 .

[29]  Abhoyjit S Bhown,et al.  In silico screening of carbon-capture materials. , 2012, Nature materials.