The　silicalite-1/PDMS　hybrid　membranes　have　been　widely　studied　in　alcohol　perm-selective　pervaporation　separations.　However,　the　poor　compatibility　between　silicalite-1　particles　and　PDMS　has　already　rebated　the　separation　performance　of　these　hybrid　membranes.　In　this　paper,　two　approaches　were　investigated　to　improve/tune　the　compatibility　of　the　silicalite-1　particles　and　PDMS　matrix.　Firstly,　silicalite-1　crystal　particles　with　different　sizes　were　synthesized.　The　effects　of　the　particle　size　on　the　compatibility　between　silicalite-1　and　PDMS　were　investigated.　It　was　found　that　smaller　silicalite-1　crystals　(about　100　nm)　have　a　better　compatibility　with　PDMS　matrix,　thereby　an　enhanced　separation　performance　of　their　hybrid　membranes.　Subsequently,　the　surface　of　silicalite-1　particles　were　modified　through　three　kinds　of　silane　coupling　agents　with　different　functional　groups,　which　was　confirmed　to　be　feasible　in　increasing　the　compatibility　with　PDMS.　In　ethanol/water　pervaporation　separation,　a　higher　selectivity　was　achieved　in　the　PDMS　hybrid　membrane　with　TMDS-modified　small　silicalite-1　crystals.　Moreover,　silicalite-1　crystals　provide　many　separate　channels,　so　that　the　separation　performance　of　the　hybrid　membrane　has　dramatically　increased.　(C)　2014　Elsevier　Inc.　All　rights　reserved.