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Capture of Carbon Dioxide from Air and Flue Gas in the Alkylamine-Appended Metal–Organic Framework mmen-Mg2(dobpdc)
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(2)O)(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.
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Metadata
- Authors
- McDonald, T. M., Lee, W. R., Mason, J. A., Wiers, B. M., Hong, C. S., & Long, J. R.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-04-12
- Volume
- 134
- Issue
- 16
- Pages
- 7056-7065
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2130360607
- Cited by
- 1,289
- References
- 52
- FWCI
- 142.11
- Type
- journal article
- Language
- en
- Open access
- closed
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