Production of bioethanol, a renewable energy source, is limited by the costly, energy-consuming concentration processes involved. Membrane separation techniques have emerged as promising alternatives to overcome these limitations. In this study, silicalite-1 zeolite membranes with high pervaporation (PV) performance were prepared on porous tubular silica supports by a secondary growth method. The effects of the deposited seed amount on the support and synthesis parameters, namely, the tetra-n-propylammonium concentration (TPA(+)/Si), alkalinity (OH-/Si), and crystallization time, were investigated. A dense zeolite layer was formed between the typical columnar crystal layer of silicalite-1 membranes and the silica support. The PV performance was mainly dependent on the thickness of the dense layer: as the thickness increased, the separation factor increased. The silicalite-1 membrane prepared using a synthesis solution with a molar composition of 1SiO(2):0.05TPABr:0.08NaOH:75H(2)O at 433 K for 8 h exhibited the highest separation performance with a separation factor of 92 and a flux of 3.00 kg m(-2) h(-1) for 10 wt% ethanol/water mixtures at 323 K, which is the best result reported to date for tubular supports. Thus, silica supports proved to be suitable for the preparation of high-performance silicalite-1 membranes for ethanol/water mixture separation. (C) 2017 Elsevier B.V. All rights reserved.