The separation ability of CHA-type and STT-type pure silica zeolite (Si-CHA and Si-STT) membranes for H-2 purification from H-2/toluene gas mixtures was investigated. When the feed mixture gas consisting of 98 mol% H-2 and 2 mol% toluene was supplied, corresponding to the gas-phase composition after removing toluene by condensation following methylcyclohexane dehydrogenation, both membranes showed good H-2-selective permeation, resulting in a hydrogen purity of above 99.9% on the permeate side.