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Following hydrothermal synthesis process, MCM-41 was synthesized by using cetyltriethylammonium bromide as templating agent. The experimental results showed that MCM-41 with pore diameter in the range of 4-7 nm can be obtained by adjusting nSurf./nSi . It was proved that cetyltriethylammonium bromide is an effective templating agent for increasing pore diameter of molecular sieve MCM-41.