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CO2 Sorption Performance of Composite Polymer/Aminosilica Hollow Fiber Sorbents: An Experimental and Modeling Study

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† School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, Georgia 30332, United States
‡ Department of Chemical & Biochemical Engineering, Missouri University of Science & Technology, 1101 East State Street, Rolla, Missouri 65409, United States
*E-mail: [email protected]
*E-mail: [email protected]
*E-mail: [email protected]
Cite this: Ind. Eng. Chem. Res. 2015, 54, 6, 1783–1795
Publication Date (Web):January 23, 2015
https://doi.org/10.1021/ie504603h
Copyright © 2015 American Chemical Society
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    Abstract

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    The dynamic CO2 sorption performance of polymer/silica supported polyethylenimine hollow fiber sorbents (CA-S-PEI), focusing on heat and mass transport effects, is investigated experimentally and computationally during sorption of CO2 from simulated, dry flue gases. The effect of the nonisothermality on the sorption performance is investigated by varying the module materials of construction. The heat effects are minimized by using a heat conductive module case with a diameter of 0.25 in., and, accordingly, the breakthrough capacities are increased by 30% over a similar module constructed from less conductive components, thereby improving fiber sorbents utilization efficiency. The sorption kinetics in CA-S-PEI hollow fiber sorbents are investigated in terms of flow rates, module packing fraction, module length, and silica particle size. A mathematical model developed previously is successfully utilized to predict various contributions to the overall mass transfer resistance. In fiber sorbents where the amine loading is high, such as those employed here, the sorption process is found to be controlled by intraparticle mass transfer resistances. Unlike fiber sorbents based on physisorbents, the external gas diffusion resistance has minimal effects on the breakthrough capacities, as evidenced with the negligible effects of the module packing fraction on the sorption capacities. Sorption capacities are found to increase with the fiber module length as a result of self-sharpening effects. The increase of particle size increases the mass transfer resistance of the fiber sorbents as illustrated by the more diffuse CO2 breakthrough fronts in fiber modules containing bigger silica particles. The capacities in fiber sorbents with the largest silica particles exhibit the lowest sorption capacity, as expected.

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    Figure S1 shows model prediction of CO2 isotherm profiles based on Toth adsorption isothermal model. Model equations including mass balance equations and energy balance equations are included in pp S2–S5. Figure S2 shows CO2 breakthrough profiles (left) and fiber temperature profiles (right) at different flue gas flow rates; solid line without marker is the model prediction. Figure S3 presents CO2 breakthrough profiles at different packing fractions for Qfluegas = 80 sccm, and temperature profile at ϕ = 0.69; solid line without marker is the model prediction. Figure S4 shows CO2 breakthrough profiles (left) at different particle sizes and temperature profiles (right) at a particle size = 25 μm; solid line without marker is the model prediction. Figure S5 model analysis: Profiles of concentration and temperature along the length of the fiber module at time t1 and t2 at 80 sccm. Figure S6 displays model prediction of the front velocity as a function of the flue gas velocity. Figure S7 shows model analysis showing the effect of flue gas flow rate on 1/Kg at τ = 70. Figure S8 is model analysis: mass transfer resistance components of bulk PEI sites (1/Kov,bulk) for the fiber modules with packing fraction of ϕ = 0.46 and ϕ = 0.69 at τ = 40. The inset shows a zoomed view of the y-axis from 0 to 1.0. Figure S9 shows model analysis of (top) propagation of the concentration front along the 34 in. fiber length and (bottom) concentration front plotted against the normalized length scale, z′ = z/zbreak. Figure S10 compares overall mass transfer resistances in the different silica sorbents at t = 28 s. Overall resistance comparison for bulk PEI 1/Kov,bulk is plotted in the main figure and for the exposed PEI 1/Kov,exposed is plotted in the inset figure. Table S1 shows the physical properties of silica supports after impregnating PEI. Table S2 shows all parameters for estimation of ψ. All of this information is cited from ref 55. This material is available free of charge via the Internet at http://pubs.acs.org.

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