Good separation performance NaY zeolite membrane was successfully prepared on the tubular mullite support by fluoride-containing precursor synthesis gel. The fluoride source had a great influence on NaY zeolite membrane growth and separation performance for EtOH/ETBE mixture, the NaF containing precursor gel was benefit for preparing high Si/Al ratio, fine reproduction quality and long-term stable NaY zeolite membrane. Solid state 19 F MAS NMR characterization results indicated that the fluorine existed in the channel of NaY zeolite crystals. Both flux and separation factor of the NaY zeolite membrane were greatly depended on the separation temperature and composition of EtOH/ETBE mixtures. The NaY zeolite membrane presented eminent long-term stability for separating 20 wt% EtOH/ETBE mixture at 60 °C, even if the test time was prolonged to 80 h, the flux and separation factor were kept 1.30 kg m −2 h −1 and 1100.
Pervaporation performance of NaY zeolite membranes is improved by ion-exchange with di-valent nitrate salt . Different nitrate salts, including Co(NO 3 ) 2 , Mg(NO 3 ) 2 , Zn(NO 3 ) 2 , Ca(NO 3 ) 2 , Cu(NO 3 ) 2 , KNO 3 , and AgNO 3 , have great effects on the channel structure and water affinity of the NaY zeolite membrane. When the concentration of nitrate salt, ion-exchange temperature and time are 0.1 mol·L −1 , 50 °C and 2 h, the ion-exchange degree order of NaY zeolites is Ag + > K + > Ca 2+ > Zn 2+ ≫ Co 2+ > Mg 2+ . Especially, Ag + and K + cation exchange degree of NaY zeolites are achieved to 96.54% and 82.77% in this work. BET surface, total pore capacity, pore size distribution and water contact angle of the ion-exchanged NaY zeolites are all disordered by mono- and di-valent cations. Di-valent nitrate salt is favor for increasing the dehydration performance of NaY zeolite membranes by ion-exchange. When the ion-exchange solution is Zn(NO 3 ) 2 , the total flux variation and separation factor variation of the NaY membrane (M-5) are −45% and 230% for separation of 10% (mass) H 2 O/EtOH mixture by pervaporation, and the ion-exchanged membranes showed good reproducibility.
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