DDR-type zeolite membrane was synthesized on porous alpha-alumina substrate by hydrothermal treatment of a ball-milled Sigmal-1 crystal seed layer in an aluminum-free precursor solution containing 1-Adamantylamine as the structure directing agent (SDA). The as-synthesized DDR zeolite membranes were defect-free but the supported zeolite layers were susceptible to crack development during the subsequent high-temperature SDA removal process. The cracks were effectively eliminated by the liquid phase chemical deposition method using tetramethoxysilane as the precursor for silica deposits. The modified membrane was extensively studied for H-2, He, O-2, N-2, CO2, CH4, and i-C4H10 pure gas permeation and CO2/CH4 mixture separation. At 297 K and 2-bar feed gas pressure, the membrane achieved a CO2/CH4 separation factor of 92 for a feed containing 90% CO2, which decreased to 62 for a feed containing 10% CO2 with the CO2 permeance virtually unchanged at 1.8 x 10(-7) mol/m(2) s Pa regardless of the feed composition. It also exhibited an O-2/N-2 permselectivity of 1.8 at 297 K. The gas permeation behaviors of the current aluminum-containing DDR type zeolite membrane are generally in good agreement with the findings in both experimental and theoretical studies on the pure-silica DDR membranes in recent literature. (C) 2016 Elsevier B.V. All rights reserved.