Application Abstract: The structure-property relationships and adsorption mechanism of CO2 in representative MOFs were investigated by using density functional theory.The CO2 adsorption behavior in zeolitic imidazolate frameworks(ZIFs),as well as the diffusion behavior in the one-dimensional pore were investigated.The adsorption phenomena of CO2 in ZIFs at different pressure were described by grand canonical Monte Carlo(GCMC)simulations.The effect of incorporating function groups and doping metal atom on CO2 adsorption capacity at low pressure were analysised,and the effective ways to enhance CO2 capture properties by chemical modifications were presented.The adsorption behavior of CO2 in MOFs with open metal sites were further investigated,and the adsorption mechanism were detailed analysised.Strong binding site molarity was proposed to predict the CO2 adsorpiton through the comparative validation between theoretical simulation and experiament results.The screening of MOFs was performed to select the MOFs with high CO2 capture performance.The effects of water vapor and other gas impurities(such as O2,SO2,NOx)on CO2 adsorption and CO2/N2 separation were investigated by GCMC simulations.The mechanisms of these effects were also investigated by DFT calculations.The work was performed by multi-disciplinary studies of combustion science,quantum chemistry,molecular simulation and material science.The results provides base for molecular design the new nanoporous materials that satisfy the requirements of post-combustion CO2 capture.
