Schenk, MA; (1999) Design of operable reactive distillation columns. Doctoral thesis , University of London.

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Abstract

Reactive distillation is an integrated process which considers simultaneous physical and chemical transformations. It is increasingly receiving attention both from industry and academia. Significant advances have been made in the area of modelling and simulation as well as the implementation of such units industrially. However, the area of control and optimisation of such units has not been explored thoroughly. The thesis presents a general framework for simulation and design, which can handle reactive and non-reactive systems. Various different aspects of the modelling and simulation of distillation have been described in order to understand the behaviour of the reactive distillation columns. In the framework both simulation modes, steady-state and dynamic, are considered and the process is described by equilibrium and non equilibrium-based models. In a rate-based (or non equilibrium) model, mass transfer rates between liquid and vapour phase are considered explicitly, based on the Maxwell-Stefan equations. Equilibrium is attained at the phase interface in the non-equilibrium model. A switching policy makes it possible to go from one model to the other, based on the knowledge gained, by following the Gibbs free energy as a function of time. Tray efficiency has also helped in determining the switch between the non-equilibrium and equilibrium models, and has been studied for various systems. The existence of multiple steady state has been verified through simulation with the hybrid model. Bifurcation diagrams also confirmed the existence of output multiplicity obtained in the simulations. Analysis of process controllability at the design stage has been shown to provide guidance for improving process operation. In the thesis controllability measures for the reactive systems studied are presented as a first step towards control structure selection. A method for obtaining the design of reactive separation columns at minimum total annualised cost (investment and operating costs) and which will be able to maintain stable operation in the presence of variability is also presented.

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