Pervaporation of organic/water mixtures by MFI type zeolite membranes synthesized in a flow system


Thesis Type: Postgraduate

Institution Of The Thesis: Orta Doğu Teknik Üniversitesi, Faculty of Engineering, Department of Chemical Engineering, Turkey

Approval Date: 2007

Student: ÖZLEM DEDE

Supervisor: HALİL KALIPÇILAR

Abstract:

Zeolite membrane synthesis is conventionally carried out in batch systems. Recently, several attempts have been performed to synthesize zeolite membranes in flow systems which can allow preparation of membranes with large specific surface areas. Membranes synthesized in the recirculating flow system had comparable N2/SF6 and n- C4H10/i-C4H10 ideal selectivities with the membranes prepared in the batch system, indicating that good quality membranes can be produced by this method. The objective of this study is to separate organic/water mixtures by pervaporation by using MFI type membranes synthesized in the flow system. Effect of number of synthesis steps and synthesis method on the separation factor and flux was investigated. Membranes were synthesized from clear solutions with a molar composition of 80SiO2:16TPAOH:1536H2O at 95oC and atmospheric pressure. The synthesis solution was recirculated through the tubular alumina support with a flow rate of 6 ml/min for 72 h. The membranes were characterized by X-ray diffraction for phase identification and scanning electron microscopy for morphology determination. Single gas permeances of N2, H2, CH4, CO2, n-C4H10 and i-C4H10 were measured between 25 and 200oC. Mixtures of 5 wt% ethanol/water, 2-propanol/water and acetone/water were separated by pervaporation at different temperatures. The single gas permeances decreased with increasing temperature for weakly adsorbed gases. For n-C4H10 the permeance passed through a maximum and i-C4H10 permeance was nearly constant. For a membrane synthesized by two consecutive synthesis steps, the ideal selectivity for n-C4H10/i-C4H10 was 132 at 200oC. The selectivity in the pervaporation separation of ethanol-water mixture was 43 with a permeate flux of 0.2 kg/m2h at 25oC. With increasing temperature, selectivity decreased but the flux increased, the selectivity was 23 and the flux was 1.9 kg/m2h at 85oC. 2-propanol/water and acetone/water separation factors were 36 and 1024 with 0.2 and 0.1 kg/m2h fluxes, respectively. The separation factors and fluxes for membranes synthesized in the flow system were comparable with membranes synthesized in the batch system.