采用十六烷基三甲基溴化铵(CTAB)-NaOH混合溶液对HZSM-35分子筛进行碱处理,并采用XRD、XRF、N2物理吸附-脱附、NH3-TPD、Py-IR、TPO手段对碱处理HZSM-35分子筛进行表征,同时将其应用于催化二甲醚(DME)羰基化反应。结果表明,采用NaOH浓度在0.1~0.6 mol/L范围的CTAB-NaOH混合溶液碱处理HZSM-35分子筛,可部分脱除HZSM-35分子筛微孔孔道内的无定形硅铝物种,提高其八元环的总酸量,使其在催化DME羰基化反应时的DME转化率(64.4%)比未碱处理(50.0%)和单独NaOH碱处理者(54.9%)均有一定程度的提高,同时有效地抑制了催化剂上积炭的生成,但乙酸甲酯选择性变化不明显。碱处理HZSM-35在DME羰基化反应中的催化性能不仅与其八元环的总酸量有关,而且还与其孔道扩散性能相关。
Alkali treatment with hexadecyl trimethyl ammonium bromide(CTAB)-NaOH solution was applied to HZSM-35 zeolites.The alkali-treated HZSM-35 samples were characterized by XRD,XRF,N2adsorption-desorption,NH3-TPD,Py-IR,TPO and used as catalyst for dimethyl ether(DME)carbonylation.The results showed that catalyzed by the alkali-treated ZSM-35 with the CTAB-NaOH solutions of 0.1-0.6mol/L NaOH,higher DME conversion of DME carbonylation and lower coke deposition on catalyst were observed,compared to the DME carbonylation catalyzed by the parent and the alkali-treated sample with only NaOH,except methyl acetate selectivity unchanged,which was ascribed not only to the removal of amorphous species from the zeolite channel and the increment of acid amount in eight-membered rings of HZSM-35 after the alkali treatment,but also to the diffusion properties of HZSM-35.