| Autor: |
Siegelman RL, Milner PJ, Forse AC, Lee JH, Colwell KA, Neaton JB; Kavli Energy Nanosciences Institute at Berkeley , Berkeley , California 94720 , United States., Reimer JA, Weston SC; Corporate Strategic Research , ExxonMobil Research and Engineering Company , Annandale , New Jersey 08801 , United States., Long JR |
| Jazyk: |
angličtina |
| Zdroj: |
Journal of the American Chemical Society [J Am Chem Soc] 2019 Aug 21; Vol. 141 (33), pp. 13171-13186. Date of Electronic Publication: 2019 Aug 08. |
| DOI: |
10.1021/jacs.9b05567 |
| Abstrakt: |
Supported by increasingly available reserves, natural gas is achieving greater adoption as a cleaner-burning alternative to coal in the power sector. As a result, carbon capture and sequestration from natural gas-fired power plants is an attractive strategy to mitigate global anthropogenic CO 2 emissions. However, the separation of CO 2 from other components in the flue streams of gas-fired power plants is particularly challenging due to the low CO 2 partial pressure (∼40 mbar), which necessitates that candidate separation materials bind CO 2 strongly at low partial pressures (≤4 mbar) to capture ≥90% of the emitted CO 2 . High partial pressures of O 2 (120 mbar) and water (80 mbar) in these flue streams have also presented significant barriers to the deployment of new technologies for CO 2 capture from gas-fired power plants. Here, we demonstrate that functionalization of the metal-organic framework Mg 2 (dobpdc) (dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) with the cyclic diamine 2-(aminomethyl)piperidine (2-ampd) produces an adsorbent that is capable of ≥90% CO 2 capture from a humid natural gas flue emission stream, as confirmed by breakthrough measurements. This material captures CO 2 by a cooperative mechanism that enables access to a large CO 2 cycling capacity with a small temperature swing (2.4 mmol CO 2 /g with Δ T = 100 °C). Significantly, multicomponent adsorption experiments, infrared spectroscopy, magic angle spinning solid-state NMR spectroscopy, and van der Waals-corrected density functional theory studies suggest that water enhances CO 2 capture in 2-ampd-Mg 2 (dobpdc) through hydrogen-bonding interactions with the carbamate groups of the ammonium carbamate chains formed upon CO 2 adsorption, thereby increasing the thermodynamic driving force for CO 2 binding. In light of the exceptional thermal and oxidative stability of 2-ampd-Mg 2 (dobpdc), its high CO 2 adsorption capacity, and its high CO 2 capture rate from a simulated natural gas flue emission stream, this material is one of the most promising adsorbents to date for this important separation. |
| Databáze: |
MEDLINE |
| Externí odkaz: |
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