Modeling adsorption of organic compounds on activated carbon a multivariate approach

Abstract: Activated carbon is an adsorbent that is commonly used for removing organic contaminants from air due to its abundant pores and large internal surface area. This thesis is concerned with the static adsorption capacity and adsorption kinetics for single and binary organic compounds on different types of activated carbon. These are important parameters for the design of filters and for the estimation of filter service life. Existing predictive models for adsorption capacity and kinetics are based on fundamental “hard” knowledge of adsorption mechanisms. These models have several drawbacks, especially in complex situations, and extensive experimental data are often needed as inputs. In this work we present a systematic approach that can contribute to the further development of predictive models, especially for complex situations. The approach is based on Multivariate Data Analysis (MVDA), which is ideally suited for the development of soft models without incorporating any assumptions about the mathematical form or fundamental physical principles involved.Adsorption capacity and adsorption kinetics depend on the properties of the carbon and the adsorbate as well as experimental conditions. Therefore, to make general statements regarding adsorption capacity and kinetics it is important for the resulting models to be representative of the conditions they will simulate. Accordingly, the first step in the investigations underlying this thesis was to select a minimum number of representative and chemically diverse organic compounds. The next steps were to study the dependence of the derived affinity coefficient, β, in the Dubinin-Radushkevich equation on properties of organic compounds and to establish a new, improved model. This new model demonstrates the importance of adding descriptors for the specific interaction with the carbon surface to the size and shape descriptors. The adsorption capacities of the same eight organic compounds at low relative pressures were correlated with compound properties. It was found that different compound properties are important in the various stages of adsorption, reflecting the fact that different mechanisms are involved. Ideal adsorbed solution theory (IAST) in combination with the Freundlich equation was developed to predict the adsorption capacities of binary organic compound mixtures. A new model was proposed for predicting the rate coefficient of the Wheeler-Jonas equation which is valid for breakthrough ratios up to 20%. Finally, it was shown that the Wheeler-Jonas equation can be adapted to describe the breakthrough curves of binary mixtures. New models were proposed for predicting its parameters, the adsorption rate coefficients, and the adsorption capacities for both components of the binary mixture. Thus, multivariate data analysis can not only be used to assist in the understanding of adsorption mechanisms, but also contribute to the development of predictive models of adsorption capacity and breakthrough time for single and binary organic compounds.