Breakthrough analysis for parameter estimation of CO2 adsorption on pelletized flexible metal-organic framework

Pellets of elastic layer-structured metal-organic framework-11 (ELM-11), one of the flexible metal-organic frameworks (MOFs), were prepared by mixing ELM-11 powder with a cellulose binder, and the CO2 adsorption behavior of ELM-11 pellets in a fixed-bed adsorber was analyzed to estimate equilibrium and kinetic parameters. Adsorption breakthrough tests were performed under various conditions for the simulated flue gas (20 % CO2-80 % N2) of a blast furnace gas in addition to CO2 isotherm measurements. Experimental CO2 adsorption isotherms on ELM-11 followed a weighted dual-site Langmuir equilibrium model well. The breakthrough analysis results by numerical calculation using the equilibrium model suggested that the gate-opening pressure of ELM-11 shifted to a lower pressure through repeated breakthrough tests. The CO2 adsorption kinetics on ELM-11 pellets agreed well with the linear-driving-force model. Furthermore, CO2 adsorption behavior under various conditions was described well by a mathematical model using a constant value of the mass transfer coefficient under the condition of this study, which was validated against additional experimental data. In addition, it was found that the mass transfer becomes slow under certain conditions that the driving force of the phase transition of ELM-11 is smaller than a threshold, where the amount of CO2 adsorbed on the breakthrough tests did not reach the equilibrium capacity of CO2, which may because the rate-limiting step may be dependent on the CO2 partial pressure and temperature.