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    A Multiscale Study of MOFs as Adsorbents in H2 PSA Purification
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    Institute for Materials and Processes, School of Engineering, The University of Edinburgh, Sanderson Building, The King’s Buildings, Mayfield Road Edinburgh EH9 3JL, U.K.
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    Industrial & Engineering Chemistry Research

    Cite this: Ind. Eng. Chem. Res. 2013, 52, 29, 9946–9957
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    https://doi.org/10.1021/ie4011035
    Published June 17, 2013
    Copyright © 2013 American Chemical Society
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    Abstract

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    In this multiscale study, four robust zirconium oxide based metal–organic frameworks (MOFs) were examined using powerful molecular simulation tools as well as indispensable full-scale PSA system modeling to determine their potential for H2 purification. Grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations were employed to evaluate the MOF working capacities, binary-mixture selectivities, and micropore transport diffusivities for each of the components of a steam methane reformer offgas (SMROG) stream: H2, CO, CH4, N2, and CO2. The small, functionalized pores of UiO-66(Zr)-Br were found to result in high N2 and CO selectivities and working capacities, whereas the slightly larger pore volume of UiO-66(Zr) favored higher CO2 and CH4 working capacities. The collective impact of impurity uptakes and selectivities on the purification of H2 from five-component steam methane reformer offgas mixtures was investigated through PSA column modeling. The breakthrough behavior of SMROG mixtures in columns containing MOF crystallites was determined using the simulated adsorption and diffusivity data as input. MOF breakthrough curves for single and two-layered beds were compared to those of commercial adsorbents including Zeolite 5A and Calgon PCB. Two of the MOFs, namely, UiO-66(Zr) and UiO-66(Zr)-Br, were found to have longer dimensionless breakthrough times than the commercial zeolite materials and are therefore expected to result in larger yields of high-purity H2 per PSA cycle. UiO-66(Zr)-Br was found to be the most promising of the four MOFs, having the longest dimensionless breakthrough times in both single and two-layered bed setups.

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    Supporting Information

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    Calculation of micropore and macropore diffusion parameters and linear driving force parameters for micropore and macropore diffusion (Table S1). EF-NEMD simulation details. Breakthrough model and simulation details. Process parameters adopted in the PSA column simulations (Table S2). Dual-site Langmuir parameters for the four MOFs, zeolites, and activated carbons (Tables S3–S5). Validation of breakthrough simulations and comparison of simulated and experimental breakthrough curves (Figure S1). Validation of adsorption isotherm simulations for UiO-66(Zr) (Figure S2). MOF working capacities for pressure ranges equivalent to the impurity partial pressures in SMROG (Figures S3 and S4, Table S6). Isosteric heats of adsorption for each of the MOFs as a function of loading (Figures S5–S8). Estimated bulk densities of the four MOFs studied (Table S7). This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: Ind. Eng. Chem. Res. 2013, 52, 29, 9946–9957
    Click to copy citationCitation copied!
    https://doi.org/10.1021/ie4011035
    Published June 17, 2013
    Copyright © 2013 American Chemical Society
    Request reuse permissions

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