Halogen-assisted conversion of lower alkanes

A method for converting methane to higher molecular weight hydrocarbons, said method comprising the steps of:

• contacting a first reaction mixture comprising methane, HCl and an oxygen-containing gas with a first catalytic composition comprising crystalline copper aluminum borate, having the significant X-ray diffraction pattern set forth in Table A, at appropriate reaction conditions to form an intermediate composition comprising chloromethane;
• and
• contacting said chloromethane with a second catalytic composition under appropriate reaction conditions to form hydrocarbon products having molecular weights greater than said methane, said second catalytic composition comprising crystalline borosilicate and a porous refractory inorganic oxide, said borosilicate and said inorganic oxide having been intimately admixed with one another, said borosilicate comprising a molecular sieve material having the following composition in terms of mole ratios of oxides:
• 0.9.+-.0.2 M.sub.2/n O:B.sub.2 O.sub.3 :ySiO.sub.2 :zH.sub.2 O
• wherein M is at least one cation having a valence n, y is between 4 and about 600, and z is between 0 and about 160 and having the significant X-ray diffraction pattern set forth in Table II.

A method for converting methane to higher molecular weight hydrocarbons, said method comprising the steps of:

• contacting a reaction mixture comprising methane, HCl and an oxygen-containing gas with a first catalytic composition comprising crystalline copper aluminum borate and a promoting amount of alkali metal compound, said first catalytic composition having the significant X-ray diffraction pattern set forth in Table A and having a surface area in the range of about 0.1 to about 300 m.sup.2 /g, under appropriate conditions to form an intermediate composition comprising chloromethane, wherein said chloromethane comprises methyl chloride, and water;
• and
• contacting said methyl chloride with a second catalytic composition under appropriate conditions to form a product stream comprising hydrocarbons having a higher molecular weight than methane, said second catalytic composition comprising crystalline borosilicate, a porous refractory inorganic oxide and additionally comprising a promoter material of at least one element selected from the group consisting of iron and gallium, said borosilicate and said inorganic oxide having been intimately admixed with one another, said borosilicate comprising a molecular sieve material having the following composition in terms of mole ratios of oxides:
• 0.9.+-.0.2 M.sub.2/n O:B.sub.2 O.sub.3 :ySiO.sub.2 :zH.sub.2 O
• wherein M is at least one cation having a valence n, y is between 4 and about 600, and z is between 0 and about 160 and having the significant X-ray diffraction pattern set forth in Table II.