A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism

Milner, Phillip J.; Siegelman, Rebecca L.; Forse, Alexander C.; Gonzalez, Miguel I.; Runčevski, Tomče; Martell, Jeffrey D.; Reimer, Jeffrey A.; Long, Jeffrey R.

doi:10.1021/jacs.7b07612

A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO₂ Capture from Coal Flue Gas via a Mixed Adsorption Mechanism

Journal Article · Thu Sep 14 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b07612· OSTI ID:1464144

Milner, Phillip J. ^[1]; Siegelman, Rebecca L. ^[1]; Forse, Alexander C. ^[2]; Gonzalez, Miguel I. ^[1]; Runčevski, Tomče ^[3]; Martell, Jeffrey D. ^[1]; Reimer, Jeffrey A. ^[1]; ^[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)

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) (dobpdc^4-= 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 (Δh_ads= -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO₂ adsorption (Δs_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-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.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: Exxonmobil Research and Engineering Company (EMRE); National Inst. of Health (NIH); Philomathia Foundation; USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0001015

OSTI ID:: 1464144

Alternate ID(s):: OSTI ID: 1406619

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 38 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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