Control of Methane Chlorination with Molecular Chlorine Gas using Zeolite Catalysts: Effects of Si/Al Ratio and Framework Type

•CH4 chlorination with Cl2 is investigated using zeolites with various Si/Al ratios.•Aluminum in the zeolite framework is a catalytic site for selective production of CH3Cl.•CH3Cl yield increased in proportional to the amount of aluminum in zeolites.•CH3Cl yield can be achieved to above 20 % at GHSV of 2400 cm3 gcat−1 h−1 at 350 °C.