NEW-PMR · New Frontiers in (Trans)esterification Pervaporation Membrane Reactors

New Frontiers in (Trans)esterification Pervaporation Membrane Reactors

The project New Pervaporation Membrane Reactor (New-PMR) has provided groundbreaking research on the development, application and modelling of (trans)esterification pervaporation membrane reactors. Pervaporation membrane reactors (PMRs) integrate the reaction and separation steps and it is a recognized concept that provides significant synergetic effects, so that a drastic improvement of the performance of the reactor is obtained. PMRs have been applied successfully for equilibrium-limited reactions involving water as one of the side products. However, the fundamentals and feasibility of this integrative approach had not yet been demonstrated for chemical conversions yielding an organic by-product such as methanol or ethanol. This project has provided a scientific basis for this and this report shows the main results obtained during the project execution. The reference reaction between butanol and methyl acetate to produce methanol and butyl acetate is deeply studied in this project. In addition, the study has been extended to other transesterification reactions, i.e., the reaction between methanol and ethyl acetate to produce ethanol and methyl acetate, which is a reference reaction in biodiesel production; production of methyl tert-butyl ether (MTBE). Experimental results with commercial membranes have demonstrated the capability of some membranes to separate butanol from the reaction medium due to a higher permeance of this component through the membrane. Using those membranes in an industrial schema would reduce the energy of separation considerably since the azeotrope between butanol and butyl acetate is not an issue if pervaporation is used prior to distillation. The potential of these membranes allocates them as a very attractive solution in combination with distillation of in a cascaded approach. In addition, a deep experimental study for multicomponent mixtures have demonstrated the critical importance of the driving force in the separation. Most of the commercial membranes enhance the permeance of components with the lowest driving force, indicating that the membrane is acting against the natural tendency of separation based on thermodynamics. This behavior may have a negative effect on the economics of the process since the permeate become less pure and the separation is not working under optimal conditions. A clear methodology to determine the performance of the separation has been proposed. Pervaporation has been integrated in conventional processes in combination with distillation and as stand-alone technology, and the applicability of several flowsheets has been determined. It was estimated that performing the separation of methanol-methyl acetate using pervaporation requires over 90% less energy to the utilities in comparison with distillation. Also, in addition to pervaporation, the alternative use of membrane contactors for the specific case of purification of biodiesel has been evaluated. Life cycle assessment analyses have been also performed together with exergy analyses. The integration of membrane technology in a hybrid configuration (i.e. pervaporation-distillation) has shown advantages to be considered in the design and development of more environmentally friendly processes (e.g., processes involving azeotropic mixtures such as those that appear in transesterification reactions). A guideline based on the impact during the production stage of the main solvents used in the chemical industry has been also developed. This guideline allows the selection of the best environmentally friendly treatment depending on the composition of the liquid mixture. Incineration (heat recovery) versus distillation (material recovery) represents the technological alternatives. The CIG Marie Curie Grant has initiated a new research line at the Université catholique de Louvain that continues after the termination of the Grant. Thanks to the impulse given by the grant, I have developed my own independent research as professor at the Université catholique de Louvain (UCL in Louvain-la-Neuve, Belgium).

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