Continuous countercurrent deterpenation of lemon essential oil by means of supercritical carbon dioxide: Experimental data and process modelling

Abstract

A thermodynamic model based on the Peng–Robinson equation of state was developed in order to perform high-pressure phase equilibria calculations for the system carbon dioxide–lemon essential oil. The multicomponent natural oil was simulated by a mixture of three key components, one for each relevant class of compounds (monoterpenes, monoterpene oxygenated derivatives and sesquiterpenes). Firstly the proposed model was validated on semi-batch experimental data and then it was used to simulate the behaviour of a continuously operated countercurrent column. Experiments on deterpenation process on a packed column, operating as a stripping section, were carried out in the temperature range 50–70 °C and pressure range 8.7–11.2 MPa. The comparison between experimental results and process simulation demonstrated that the proposed model is capable of reliable predictions on the behaviour of the countercurrent continuous deterpenation process. Furthermore, an average height equivalent to a theoretical plate of about 40 cm was estimated, for the stated packing and operating conditions. A case study for the production of 10-fold high quality oil, with strict specifications for the recovery of oxygenated compounds (99%), was investigated by simulations of a continuous countercurrent process with an external reflux. The linkage between the number of theoretical stages, the reflux ratio and the solvent to feed ratio was investigated throughout the above-mentioned pressure and temperature ranges. Operating conditions at higher pressure and temperature proved to be more favourable. As an example, operating a 20 theoretical stage column at 70 °C and 11.2 MPa, it is possible to attain process specifications with a solvent to feed ratio of about 63.