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Dirk Otter
Adsorption on Metal-Organic Frameworks
From Material Characterization to CO2/CH4 Separation
This manuscript contains the research results of four comprehensive and peer-reviewed articles on the topic of gas-phase adsorption and grants full access to the related MATLAB codes for the modelling and simulation of adsorption equilibria as well as dynamic adsorption, both for multicomponent mixtures (see download section).
A novel isostructural series of metal-organic frameworks, IFP, is characterised with respect to its separation properties for CO₂ /CH₄ mixtures. The highly microporous materials are analysed both in terms of their morphological and structural properties in static adsorption screenings (equilibrium measurements) as well as their separation behaviour in dynamic adsorption processes in fixed beds (breakthrough curves). In this context the influence of different functional groups on the physicochemical properties of the isoreticular IFP series is also highlighted.
The mathematical models for describing static and dynamic adsorption are presented and validated on basis of experimental data, including a new model for the description of hysteresis exhibiting water vapour isotherms, as well as for adsorption equilibria of pure substances and mixtures, and in particular a model for the simulation of non-isothermal breakthrough curves taking into account the mass and heat balances, respectively. By applying a heterogeneous kinetic model, detailed kinetic analyses are performed on the experimental data and the importance of kinetically induced selectivity enhancement is illuminated.
On basis of this insight a core-shell composite material consisting of affordable mesoporous alumina carriers coated with more expensive but kinetically selective Ni-MOF-74 is used to demonstrate an increase in separation efficiency allowing economically more viable processes.
A novel isostructural series of metal-organic frameworks, IFP, is characterised with respect to its separation properties for CO₂ /CH₄ mixtures. The highly microporous materials are analysed both in terms of their morphological and structural properties in static adsorption screenings (equilibrium measurements) as well as their separation behaviour in dynamic adsorption processes in fixed beds (breakthrough curves). In this context the influence of different functional groups on the physicochemical properties of the isoreticular IFP series is also highlighted.
The mathematical models for describing static and dynamic adsorption are presented and validated on basis of experimental data, including a new model for the description of hysteresis exhibiting water vapour isotherms, as well as for adsorption equilibria of pure substances and mixtures, and in particular a model for the simulation of non-isothermal breakthrough curves taking into account the mass and heat balances, respectively. By applying a heterogeneous kinetic model, detailed kinetic analyses are performed on the experimental data and the importance of kinetically induced selectivity enhancement is illuminated.
On basis of this insight a core-shell composite material consisting of affordable mesoporous alumina carriers coated with more expensive but kinetically selective Ni-MOF-74 is used to demonstrate an increase in separation efficiency allowing economically more viable processes.
Schlagwörter: Multicomponent Adsorption; Adsorption Equilibria; IAST; RAST; Isotherm Hysteresis; Dynamic Adsorption; Adsorption Kinetics; Fixed Bed; Breakthrough Curve; Core-Shell; MOF; Matlab; Simulation; Modelling; Carbon Capture; Gas Separation; Biogas; Natural Gas
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