CTAB-NaOH混合液碱处理HZSM-35分子筛催化DME羰基化反应  

Dimethylether Carbonylation Over ZSM-35 Zeolites Alkali-Treated With CTAB-NaOH Solution

作　　者：刘小行 刘盛林[1] 李秀杰[1] 谢素娟[1] 徐龙伢[1] 曾蓬[3] 赵明军 

机构地区：[1]中国科学院大连化学物理研究所,辽宁大连116023 [2]中国科学院大学,北京100049 [3]中国寰球工程公司辽宁分公司,辽宁抚顺113006 [4]中国石油抚顺石化分公司,辽宁抚顺113004

出　　处：《石油学报（石油加工）》2014年第6期967-975,共9页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(21376235)资助

摘　　要：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.

关 键 词：二甲醚 羰基化 十六烷基三甲基溴化铵 ZSM-35 碱处理 

分 类 号：TQ426.96[化学工程]