A General Framework Linking Adsorbent Characterization and Process Simulation: Kinetics, Isotherms, and Adsorption Bed Modeling

Author(s)
Wu, Mengjiao
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School of Chemical and Biomolecular Engineering
School established in 1901 as the School of Chemical Engineering; in 2003, renamed School of Chemical and Biomolecular Engineering
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Abstract
This dissertation presents an integrated framework that combines material characterization, numerical modeling, data-driven analysis, and adsorption-bed simulation to evaluate novel adsorbents for adsorption-based separation processes. A modeling approach was developed to extract adsorption kinetic parameters directly from dynamic gravimetric and volumetric experiments, eliminating restrictive assumptions of traditional analytical solutions and providing accurate diffusivities and mass transfer coefficients across diverse materials. To incorporate complex mixture adsorption behavior into process simulations, a symbolic regression method was created to generate empirical gas mixture isotherm equations from discrete experimental or molecular simulation data, with numerical stability filtering enabling reliable implementation during adsorption bed modeling. These equations were successfully used in breakthrough simulations to predict mixture adsorption dynamics in systems where classical models or IAST are insufficient. An efficient adsorption bed simulation toolbox was further developed using numerical quadrature for discrete isotherms, a high-order WENO scheme for breakthrough modeling, and pre-generated isotherm grids with spline interpolation to eliminate repeated IAST calculations and improve computational speed. The framework was demonstrated through a case study on atmospheric water harvesting with LiCl-impregnated MIL-101 analogs, showing that although higher salt loadings increase water uptake, LiCl induced mass transfer limitations slow kinetics and constrain rapid cycling, while higher gas flow velocities partially mitigate these effects. Overall, this work provides a flexible and computationally efficient pathway for translating laboratory-scale adsorption measurements into process-level performance predictions.
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Date
2025-12
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Text
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Dissertation (PhD)
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