Adsorption And Chemical Equilibria On Porous Materials By Molecular Simulation And Separation Of CH₄/CO₂ By Experiment And Modeling

This thesis contains two relatively independent parts, i.e. chemical equilibria of complicated systems confined in porous materials and adsorption separation of methane and carbon dioxide on activated mesocarbon microbeads (a-MCMBs).In part one, the chemical equilibria of three important reactions in porous materials were simulated by Reactive Canonical ensemble Monte Carlo (RCMC) method, to understand chemical equilibrium in nano-scale confinement.a-MCMBs is a promising adsorbent for methane storage. Accordingly, in part two, the combine method 'experiment characterization-equation of state (EOS) theory analysis-molecular simulation technology' was used to study adsorption separation of carbon dioxide and methane on a-MCMBs. The investigation provides valuable guidance and points of reference for the development of new absorbents and new adsorption materials. The main contents and findings are summarized as follows.Aimed at two important meso-porous materials of MCM-41 and pillared clays in catalytic filed, RCMC simulation was firstly performed to study the chemical equilibrium of ammonia synthesis confined in these media. The simulation results demonstrate that,(1) It is usually acknowledged that the molecular number density of pore phase is higher than that of bulk phase for the reason of confinement. According to Le Chatelizer principle, the increase of density of fluid would result in a corresponding increase of ammonia production in pore phase, for ammonia synthesis which has a decrease of mole number after reaction.(2) By analyzing the structural discrepancy between pillared clays and slit pores, the exceptional phenomenon that why a pillared clay with a larger pore width of 1.70 nm has a greater ammonia mole fraction in pore phase than that of a slit pore with 1.50 nm is explained satisfactorily.(3) On the conditions of low temperature of 573 K, small pore size (1.5 nm for MCM-41 and 1.02 nm for pillared clays), high pressure of 600 bar and high feed mole ratio of N:H of 4:12 (0.3333), greater ammonia mole fraction in pore phase can be obtained, whereas only at low pressure of 100 bar can achieve a more...