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Composite membranes suitable for separating gas mixtures are made by in situ crosslinking of aminoorganofunctional polysiloxane, 1 to 9 mol percent aminosiloxane units, with diisocyanate on the surface of a highly porous polymer substrate, such as polysulfone. Using the crosslinked polysiloxane as a

Composite membranes suitable for separating gas mixtures are made by in situ crosslinking of aminoorganofunctional polysiloxane, 1 to 9 mol percent aminosiloxane units, with diisocyanate on the surface of a highly porous polymer substrate, such as polysulfone. Using the crosslinked polysiloxane as a gutter layer, a gas separating entity can be coated on the gutter layer to make a double layer composite membrane which has a higher separation factor than the crosslinked polysiloxane and can be used effectively for flat sheet membranes, as well as, hollow fiber membranes.

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A method for making a composite suitable for increasing the oxygen gas content of an oxygen-nitrogen gas mixture by passing the mixture through the composite, consisting essentially of coating an aminoorganofunctional polysiloxane on at least one surface of a 20 to 250 m0.1 m20 m1 to 9 mol percent a

A method for making a composite suitable for increasing the oxygen gas content of an oxygen-nitrogen gas mixture by passing the mixture through the composite, consisting essentially of coating an aminoorganofunctional polysiloxane on at least one surface of a 20 to 250 m0.1 m20 m1 to 9 mol percent aminosiloxane units having primary aminoorganofunctionality and 91 to 99 mol percent other repeating siloxane units contacting the polysiloxane coated on the substrate with a solution of a non-isocyanate-reactive organic solvent and diisocyanate for a sufficient time to cause a crosslinked membrane to form, where the weight ratio of the polysiloxane to the diisocyanate is in an inverse relationship to the permeability coefficient of the composite. A double layer composite membrane suitable for separating gases consisting essentially of a 20 to 250 m1 to 9 mol percent primary aminoorganofunctionality bearing siloxane units and 91 to 99 mol percent other siloxane units, and tightly adhered and overcoating the gutter layer is a gas separating entity.