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combination of two factors: (1) absorption or adsorption selectivity and (2) diffusion selectivity. For optimum separation both these factors need to complement each other. CURRENT STATUS Sorption selectivity depends on the thermodynamic equilibrium between the bulk gas phase mixture and the liquid, polymeric, or crystalline solid material, whereas diffusion selectivity is dictated by the rates of transport of guest molecules within the host material. Both sorption and diffusion selectivities are dependent on a variety of factors such as the distribution of active sites, framework charges, presence of cations, pore size, pore topology, and connectivity. For ordered crystalline microporous materials such as zeolites (crystalline aluminosilicates), carbon nanotubes (CNTs), and MOFs, there is a wide variety of channel sizes, topologies, and connectivities, as illustrated in Figure 32. Reliable estimations of phase equilibria, in combination with mixture diffusion, are an essential requirement for process development and design. In practice, such estimations are not possible purely on the basis of experiments because mixture isotherms and diffusivities are more difficult to access experimentally. Use of molecular simulation techniques such as Monte Carlo, simulations in the grand-canonical ensemble, molecular dynamics, kinetic Monte Carlo, and transition state theory offer potent alternatives. However, the data accruing from such simulations need coarse-graining to obtain parameters required for use in more commonly used continuum models for describing mixture adsorption and diffusion, such as the ideal adsorbed solution theory and the Maxwell-Stefan diffusion formulation. At present, only for ordered perfect crystalline materials with rigid structures, such as zeolites and MOFs, can these thermodynamic and transport properties be predicted with a reasonable degree of confidence. LTL Mn-FA 1D channels CNT PCN -19 1D channels + side pockets MOR Side pockets cages + narrow windows DDR cavities + large windows FAU Intersecting channels ISV Figure32. Examplesofthevarietyofchanneltopologiesandconnectivitiesinzeolites,metaloxide frameworks, and carbon nanotubes. Source: Reprinted with permission from R. Krishna, “Describing the diffusion of guest molecules inside porous structures,” J. Phys. Chem. C 113, 19756–19781 (2009). Copyright 2009 American Chemical Society, where abbreviations for structures in this figure are referenced. 107PDF Image | 2020 Carbon Capture
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