389070 Structural Modification of Metal Organic Frameworks for Steam Stable CO2 Adsorbents

Tuesday, November 18, 2014: 1:50 PM
International 3 (Marriott Marquis Atlanta)
Dinara Andirova1, Yu Lei1 and Sunho Choi2, (1)Chemical Engineering, Northeastern University, Boston, MA, (2)Chemical Engineering, Northeastern University

The heightened global concern over increasing CO2 concentrations in the atmosphere have led to intensive research on CO2 mitigation strategies, specifically on the ways to capture CO2 from post-combustion flue gas. Porous adsorbent materials may represent promising pathway to capture the greenhouse gas in a simple and cost-efficient way.1 Among adsorbents, metal organic frameworks (MOFs) featuring high surface areas and chemical tunability have demonstrated competitive CO2 adsorption capacities under the CO2 capture conditions simulating the flue gas.2 However, most of the research employing MOFs as a CO2 adsorbent have been carried out under dry conditions, which is far from the realistic conditions. To use MOFs for practical CO2 capture applications such as for the flue gas, the material stability of MOFs under humid conditions should be evaluated.

In this work, structural changes and CO2 capture performance of MOFs was studied under humid CO2 capture conditions using accelerated steam treatment tests. Traces of structural degradation based on XRD patterns and porosity measurements as well as dramatic loss of its CO2 capture capacity was observed when the bare Mg/DOBDC was exposed to the humidity. To improve materials stability, pore surface modification with ethylene diamine groups was performed using post-synthesis functionalization procedures used in the previous work.3 Materials stability of the Mg/DOBDC under humid conditions was assessed before and after functionalization and analyzed using characterization techniques including XRD, surface area and pore size analyzer, TGA, etc. Amine functionalization was hypothesized to shield open metal sites of the framework from water molecules therefore protecting material from degradation. It was found that while some degradation occurred still, CO2 capacities were almost completely regenerated after steam treatment. 

            (1)      Choi, S.; Drese, J. H.; Jones, C. W. ChemSusChem 2009, 2, 796.

            (2)      Sumida, K.; Rogow, D. L.; Mason, J. A.; McDonald, T. M.; Bloch, E. D.; Herm, Z. R.; Bae, T. H.; Long, J. R. Chemical Reviews 2012, 112, 724.

            (3)      Choi, S.; Watanabe, T.; Bae, T.-H.; Sholl, D. S.; Jones, C. W. The Journal of Physical Chemistry Letters 2012, 3, 1136.

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