Capture of carbon dioxide from air and flue gas in the alkylamine-appended metal-organic framework mmen-Mg 2(dobpdc)

Thomas M. McDonald, Woo Ram Lee, Jarad A. Mason, Brian M. Wiers, Chang Seop Hong, Jeffrey R. Long

Research output: Contribution to journalArticle

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Abstract

Two new metal-organic frameworks, M 2(dobpdc) (M = Zn (1), Mg (2); dobpdc 4- = 4,4′-dioxido-3,3′-biphenyldicarboxylate), adopting an expanded MOF-74 structure type, were synthesized via solvothermal and microwave methods. Coordinatively unsaturated Mg 2+ cations lining the 18.4-Å-diameter channels of 2 were functionalized with N,N′-dimethylethylenediamine (mmen) to afford Mg 2(dobpdc)(mmen) 1.6(H 2O) 0.4 (mmen-Mg 2(dobpdc)). This compound displays an exceptional capacity for CO 2 adsorption at low pressures, taking up 2.0 mmol/g (8.1 wt %) at 0.39 mbar and 25 °C, conditions relevant to removal of CO 2 from air, and 3.14 mmol/g (12.1 wt %) at 0.15 bar and 40 °C, conditions relevant to CO 2 capture from flue gas. Dynamic gas adsorption/desorption cycling experiments demonstrate that mmen-Mg 2(dobpdc) can be regenerated upon repeated exposures to simulated air and flue gas mixtures, with cycling capacities of 1.05 mmol/g (4.4 wt %) after 1 h of exposure to flowing 390 ppm CO 2 in simulated air at 25 °C and 2.52 mmol/g (9.9 wt %) after 15 min of exposure to flowing 15% CO 2 in N 2 at 40 °C. The purity of the CO 2 removed from dry air and flue gas in these processes was estimated to be 96% and 98%, respectively. As a flue gas adsorbent, the regeneration energy was estimated through differential scanning calorimetry experiments to be 2.34 MJ/kg CO 2 adsorbed. Overall, the performance characteristics of mmen-Mg 2(dobpdc) indicate it to be an exceptional new adsorbent for CO 2 capture, comparing favorably with both amine-grafted silicas and aqueous amine solutions.

Original languageEnglish
Pages (from-to)7056-7065
Number of pages10
JournalJournal of the American Chemical Society
Volume134
Issue number16
DOIs
Publication statusPublished - 2012 Apr 25

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Carbon Monoxide
Flue gases
Carbon Dioxide
Carbon dioxide
Gases
Metals
Air
Adsorbents
Amines
Gas adsorption
Linings
Gas mixtures
Adsorption
Differential scanning calorimetry
Desorption
Positive ions
Experiments
Silica
Microwaves
Differential Scanning Calorimetry

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Capture of carbon dioxide from air and flue gas in the alkylamine-appended metal-organic framework mmen-Mg 2(dobpdc). / McDonald, Thomas M.; Lee, Woo Ram; Mason, Jarad A.; Wiers, Brian M.; Hong, Chang Seop; Long, Jeffrey R.

In: Journal of the American Chemical Society, Vol. 134, No. 16, 25.04.2012, p. 7056-7065.

Research output: Contribution to journalArticle

McDonald, Thomas M. ; Lee, Woo Ram ; Mason, Jarad A. ; Wiers, Brian M. ; Hong, Chang Seop ; Long, Jeffrey R. / Capture of carbon dioxide from air and flue gas in the alkylamine-appended metal-organic framework mmen-Mg 2(dobpdc). In: Journal of the American Chemical Society. 2012 ; Vol. 134, No. 16. pp. 7056-7065.
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AU - Lee, Woo Ram

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AU - Wiers, Brian M.

AU - Hong, Chang Seop

AU - Long, Jeffrey R.

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