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A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism
Open accessAbstract
A new diamine-functionalized metal–organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg 2+ sites lining the channels of Mg 2 (dobpdc) (dobpdc 4– = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate) is characterized for the removal of CO 2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn–Mg 2 (dobpdc) displays facile step-shaped adsorption of CO 2 from coal flue gas at 40 °C and near complete CO 2 desorption upon heating to 100 °C, enabling a high CO 2 working capacity (2.42 mmol/g, 9.1 wt %) with a modest 60 °C temperature swing. Evaluation of the thermodynamic parameters of adsorption for dmpn–Mg 2 (dobpdc) suggests that the narrow temperature swing of its CO 2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δ h ads = −73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO 2 adsorption (Δ s ads = −204 ± 4 J/mol·K) positioning the step in the optimal range for carbon capture from coal flue gas. In addition, thermogravimetric analysis and breakthrough experiments indicate that, in contrast to many adsorbents, dmpn–Mg 2 (dobpdc) captures CO 2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13 C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO 2 via formation of both ammonium carbamates and carbamic acid pairs, the latter of which are crystallographically verified for the first time in a porous material. Taken together, these properties render dmpn–Mg 2 (dobpdc) one of the most promising adsorbents for carbon capture applications.
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Cites
Carbon Dioxide Capture in Metal–Organic Frameworks
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Self-citationAmine Scrubbing for CO 2 Capture
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Self-citationWater Stability and Adsorption in Metal–Organic Frameworks
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Cited by
Hadjiivanov, K. I., Panayotov, D. A., Mihaylov, M. Y., Ivanova, E. Z., Chakarova, K. K., Andonova, S. M., & Drenchev, N. L. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00487 · Cited by 1,278
Porous metal-organic frameworks for gas storage and separation: Status and challenges
Li, H., Li, L., Lin, R.-B., Zhou, W., Zhang, Z., Xiang, S., & Chen, B. (2019) · EnergyChem · doi:10.1016/j.enchem.2019.100006 · Cited by 891
Data-driven design of metal–organic frameworks for wet flue gas CO2 capture
Boyd, P. G., Chidambaram, A., García-Díez, E., Ireland, C. P., Daff, T. D., Bounds, R., Gładysiak, A., Schouwink, P., Moosavi, S. M., Maroto-Valer, M. M., et al. (2019) · Nature · doi:10.1038/s41586-019-1798-7 · Cited by 885
Porous materials for carbon dioxide separations
Siegelman, R. L., Kim, E. J., & Long, J. R. (2021) · Nature Materials · doi:10.1038/s41563-021-01054-8 · Cited by 722
Self-citationUnderstanding the Effect of Water on CO2 Adsorption
Kolle, J. M., Fayaz, M., & Sayari, A. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00762 · Cited by 523
Metadata
- Authors
- Milner, P. J., Siegelman, R. L., Forse, A. C., Gonzalez, M. I., Runčevski, T., Martell, J. D., Reimer, J. A., & Long, J. R.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-09-14
- Volume
- 139
- Issue
- 38
- Pages
- 13541-13553
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2754120640
- Cited by
- 288
- References
- 76
- FWCI
- 23.63
- Type
- journal article
- Language
- en
- Open access
- green
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- Milner, P. J., Siegelman, R. L., Forse, A. C., Gonzalez, M. I., Runčevski, T., Martell, J. D., Reimer, J. A., & Long, J. R. (2017). A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.7b07612
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