We describe a straightforward and scalable fabrication of diamine-appended metal-organic framework (MOF)/polymer composite hollow fiber sorbent modules for CO capture from dilute streams, such as flue gas from natural gas combined cycle (NGCC) power plants. A specific Mg-MOF, Mg(dobpdc) (dobpdc = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate), incorporated into poly(ether sulfone) (PES) is directly spun through a conventional "dry-jet, wet-quench" method. After phase separation, a cyclic diamine 2-(aminomethyl)piperidine (2-ampd) is infused into the MOF within the polymer matrix during postspinning solvent exchange. The MOF hollow fibers from direct spinning contain as high as 70% MOF in the total fibers with 98% of the pure MOF uptake. The resulting fibers exhibit a step isotherm and a "shock-wave-shock" breakthrough profile consistent with pure 2-ampd-Mg(dobpdc). This work demonstrates a practical method for fabricating 2-ampd-Mg(dobpdc) fiber sorbents that display the MOF's high CO adsorption capacity while lowering the pressure drop during operation.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9241006 | PMC |
http://dx.doi.org/10.1021/jacsau.2c00029 | DOI Listing |
J Chem Phys
November 2024
ExxonMobil Technology and Engineering Company, Annandale, New Jersey 08801, USA.
The effect of humidity on the cooperative adsorption of CO2 from the air on amine-appended metal-organic frameworks is studied both experimentally and theoretically. Breakthrough experiments show that, at low relative humidities, there is an anomalous induction effect, where the kinetics at short times are slower than kinetics at long times. The induction effect gradually vanishes as relative humidity is increased, corresponding to an increase in CO2 adsorption rate.
View Article and Find Full Text PDFJ Am Chem Soc
March 2024
Institute for Decarbonization Materials, University of California, Berkeley, California 94720, United States.
J Phys Chem Lett
February 2024
Department of Physics, University of California, Berkeley, Berkeley, California 94720, United States.
Recent measurements [Xu, J.; 2019, 10 (22), 7044-7049] have reported temperature-dependent rates of detachment of diamine from Mg sites in diamine-appended Mg(dobpdc) [dobpdc = 4,4'-dihydroxy(1,1'-biphenyl)-3,3'-dicarboxylic] metal-organic frameworks, a process hypothesized to be a precursor for cooperative CO adsorption, leading to step-shaped isotherms or isobars. Here, we compute the rate of diamine exchange in this system for different diamines using metadynamics simulations based on a density functional theory-derived neural network potential.
View Article and Find Full Text PDFJ Am Chem Soc
January 2024
Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
Among the various metal-organic framework (MOF) adsorbents, diamine-functionalized Mg(dobpdc) (dobpdc = 4,4-dioxidobiphenyl-3,3'-dicarboxylate) shows remarkable carbon dioxide removal performance. However, applying diamine-functionalized Mg(dobpdc) in practical applications is premature because it shows persistent performance degradation under real flue gas conditions containing water vapor owing to diamine loss during wet cycles. To address this issue, we employed hydrophobic carbonate compounds to protect diamine groups in een-Mg(dobpdc) (, een = N-ethylethylenediamine).
View Article and Find Full Text PDFJ Am Chem Soc
August 2023
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California94720, United States.
Diamine-appended Mg(dobpdc) (dobpdc = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) metal-organic frameworks have emerged as promising candidates for carbon capture owing to their exceptional CO selectivities, high separation capacities, and step-shaped adsorption profiles, which arise from a unique cooperative adsorption mechanism resulting in the formation of ammonium carbamate chains. Materials appended with ,-diamines featuring bulky substituents, in particular, exhibit excellent stabilities and CO adsorption properties. However, these frameworks display double-step adsorption behavior arising from steric repulsion between ammonium carbamates, which ultimately results in increased regeneration energies.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!