Co2 ayirma için i̇yonik sivi/MOF kompozitleri: moleküler simülasyonlar ile deneylerin birleştirilmesi

CO2 adsorption and separation from flue gas and natural gas have significant environmental and industrial importance. Metal organic frameworks (MOFs) are promising adsorbent materials for CO2 adsorption and separation processes due to their extraordinary properties and customizable chemistries. Post-synthesis modification of MOFs by incorporation of ionic liquids (ILs) is a new approach to enhance gas adsorption and separation performance of MOFs. In the first part of this thesis, a computational methodology based on the state-of-the-art molecular simulations of IL/CuBTC composites composed of ILs having the same cation, 1-n-butyl-3-methylimidazole ([BMIM]+), and various anions was proposed. Using grand canonical Monte Carlo (GCMC) simulations, CO2, CH4, and N2 uptakes of seven different IL/CuBTC composites were predicted and compared with the experimental gas uptake measurements to select the most appropriate force field. Motivated from the good agreement between experiments and simulations, the same method was applied to estimate the gas adsorption in two new IL/CuBTC composites which have been synthesized and characterized for the first time in this work. Molecular simulations accurately predicted the experimental gas uptakes of newly synthesized composites, validating the transferability of the approach to different IL/CuBTC samples. A detailed analyses of binary gas mixture separation performances of IL/CuBTC composites and diffusion of gases in IL/CuBTC composites were also provided. In the second part, the computational methodology that proposed in the first part was validated using three 1-n-butyl-3-methylimidazolium tetrafluoroborate [BMIM][BF4]/MOF composites with comparable IL-loadings, one of which was synthesized and characterized for the first time in this work. This computational methodology was then used to predict the CO2/N2 binary mixture adsorption and separation performances of 1108 different [BMIM][BF4]/MOF composites. Results showed that vast majority of the [BMIM][BF4]/MOF composites exhibit increase in their CO2 adsorption and separation performances. Structural reasons behind the increased performance of IL/MOF composites were examined. The results of this thesis show that IL/MOF composites have a great potential in CO2 adsorption and separation. Results and the methodology provided in this work will be useful to assess the CO2 adsorption and separation performances of different IL/MOF composites.