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DOE OSTI · 2480569

Integrated CO 2 Capture and Conversion by a Robust Cu(I)-Based Metal–Organic Framework

Sengupta, Debabrata·Bose, Saptasree·Wang, Xiaoliang·Schweitzer, Neil M.·Malliakas, Christos D.·Xie, Haomiao·Duncan, Joshua·Kirlikovali, Kent O.·Yildirim, Taner·Farha, Omar K.
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Abstract

Metal-organic frameworks (MOFs) have shown promise in both capturing CO 2 under flue gas conditions and converting it into valuable chemicals. However, the development of a single MOF capable of capturing and selectively converting CO 2 has remained elusive due to lack of harmonious combination of selectivity, water stability, and reactivity. For example, Cu(I)-based MOFs are particularly effective for CO 2 conversion, but they do not typically exhibit selective CO 2 adsorption and often suffer from instability in the presence of air and moisture. Developing a Cu(I) MOF that is stable under flue gas conditions while also capturing CO 2 from this mixture would likely afford a material capable of selectively capturing and converting CO 2 in an integrated pathway, which would represent a significant advancement in this field. In this study, we introduce NU-2100, an ultramicroporous Cu(I) MOF, which exhibits both selectivity for CO 2 adsorption and great stability even in the presence of moisture and air. Comprehensive evaluations involving exposure to air, oxygen, water, and varying temperatures reveal that NU-2100 demonstrates superior stability compared to other known Cu(I) MOFs. Utilizing adsorption isotherms and thermogravimetric analysis coupled with gas chromatography-mass spectrometry (TGA-GCMS), we establish the high selectivity of NU-2100 for CO 2 over common flue gas components, including water, nitrogen, and oxygen. Additionally, under mild reaction conditions (50 °C and H 2 :CO 2 = 3:1), NU-2100 exhibits CO 2 capture and catalytic conversion to formic acid with 100% selectivity. Furthermore, this study marks an important step towards the design of next-generation MOFs capable of integrated carbon capture and utilization (iCCU) under industrial conditions.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYInorganic carbon compoundsMetal organic frameworksOrganic acidsOxidesStability

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Sengupta, Debabrata, Bose, Saptasree, Wang, Xiaoliang, Schweitzer, Neil M., Malliakas, Christos D., Xie, Haomiao, Duncan, Joshua, Kirlikovali, Kent O., Yildirim, Taner, Farha, Omar K.. 2024-09-20. Integrated CO 2 Capture and Conversion by a Robust Cu(I)-Based Metal–Organic Framework. https://doi.org/10.1021/jacs.4c08757

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