A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism
Abstract
Here, a new diamine-functionalized metal-organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg2+ sites lining the channels of Mg2(dobpdc) (dobpdc4-= 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn-Mg2(dobpdc) displays facile step-shaped adsorption of CO2 from coal flue gas at 40 °C and near complete CO2 desorption upon heating to 100 °C, enabling a high CO2 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-Mg2(dobpdc) suggests that the narrow temperature swing of its CO2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δhads= -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO2 adsorption (Δsads= -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-Mg2(dobpdc) captures CO2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13C NMR spectra and single-crystal X-ray diffraction structures ofmore »
- Authors:
-
[3]
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States). Berkeley Energy and Climate Inst. (BECI)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Advanced Research Projects Agency - Energy (ARPA-E); Exxonmobil Research and Engineering Company (EMRE); National Institutes of Health (NIH); Philomathia Foundation
- OSTI Identifier:
- 1464144
- Grant/Contract Number:
- AC02-05CH11231; SC0001015; F32GM120799; AC02-06CH11357; S10OD023523
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 38; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Adsorption; Cations; Coal; Humidity; Organic compounds
Citation Formats
Milner, Phillip J., Siegelman, Rebecca L., Forse, Alexander C., Gonzalez, Miguel I., Runčevski, Tomče, Martell, Jeffrey D., Reimer, Jeffrey A., and Long, Jeffrey R. A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b07612.
Milner, Phillip J., Siegelman, Rebecca L., Forse, Alexander C., Gonzalez, Miguel I., Runčevski, Tomče, Martell, Jeffrey D., Reimer, Jeffrey A., & Long, Jeffrey R. A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism. United States. https://doi.org/10.1021/jacs.7b07612
Milner, Phillip J., Siegelman, Rebecca L., Forse, Alexander C., Gonzalez, Miguel I., Runčevski, Tomče, Martell, Jeffrey D., Reimer, Jeffrey A., and Long, Jeffrey R. Thu .
"A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism". United States. https://doi.org/10.1021/jacs.7b07612. https://www.osti.gov/servlets/purl/1464144.
@article{osti_1464144,
title = {A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism},
author = {Milner, Phillip J. and Siegelman, Rebecca L. and Forse, Alexander C. and Gonzalez, Miguel I. and Runčevski, Tomče and Martell, Jeffrey D. and Reimer, Jeffrey A. and Long, Jeffrey R.},
abstractNote = {Here, a new diamine-functionalized metal-organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg2+ sites lining the channels of Mg2(dobpdc) (dobpdc4-= 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn-Mg2(dobpdc) displays facile step-shaped adsorption of CO2 from coal flue gas at 40 °C and near complete CO2 desorption upon heating to 100 °C, enabling a high CO2 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-Mg2(dobpdc) suggests that the narrow temperature swing of its CO2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δhads= -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO2 adsorption (Δsads= -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-Mg2(dobpdc) captures CO2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO2 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-Mg2(dobpdc) one of the most promising adsorbents for carbon capture applications.},
doi = {10.1021/jacs.7b07612},
journal = {Journal of the American Chemical Society},
number = 38,
volume = 139,
place = {United States},
year = {Thu Sep 14 00:00:00 EDT 2017},
month = {Thu Sep 14 00:00:00 EDT 2017}
}
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