Computer Simulation of Carbon Dioxide Adsorption and Transport in Zeolites

Abstract

The aim of this work is to investigate the adsorption and transport of CO2 in a range of zeolites and how these processes are affected by surfaces and by the presence of water.The background to the project and a review of the literature are presented in chapter 1. Chapters 2 and 3 introduce the methodology used. Firstly the description of potential models is given in chapter 2, and an overview of the computational techniques, including energy minimisation, molecular dynamics (MD) and grand canonical Monte Carlo (GCMC), is given in chapter 3.Chapter 4 describes the structures and surface of FAU, LTA, LTL, MFI and MOR, and the development and testing of the potential model using GCMC simulations to reproduce experimental isotherms and heats of adsorption.Surface effects are very important as sorbents will often have large surface area to volume ratios, therefore chapter 5 is an analysis of the effect that surfaces have on the adsorption and transport of CO2. The work uses MD simulations and focusses on faujasite, comparing the siliceous, sodium and potassium forms and the {100}, {011} and {111}surfaces.Water will usually be present in industrial waste gas streams and is likely to have an effect on the efficacy of CO2 adsorption. The final two chapters therefore present results on the effect of water on CO2 adsorption. Chapter 6 investigates the CO2 adsorption sites in a range of bulk zeolite structures and how the presence of water changes the adsorption. Chapter 7 investigates the effect of water on CO2 transport through zeolite surfaces, comparing the {100}, {010} and {001} surfaces of siliceous MFI.Finally, chapter 8 draws together the conclusions of the thesis and suggests areas for future work.

Date of Award	17 Jan 2014
Original language	English
Awarding Institution	University of Bath
Supervisor	Steve Parker (Supervisor)