甲醇脱水合成二甲醚的 Al2O3-HZSM-5 组合固体酸催化剂

 制备了可用于固定床反应器中甲醇脱水制备二甲醚的 Al2O3-HZSM-5 组合固体酸催化剂系列, 并采用 X射线衍射、扫描电镜、N2 物理吸附和氨气程序升温脱附等对其进行了表征. 结果表明, 在浸渍法制备的组合 Al2O3-HZSM-5 催化剂中, 细小的氧化铝颗粒高度分散在 HZSM-5 分子筛的周围; 在化学沉淀法制备的组合 Al2O3-HZSM-5 催化剂中, 一层氧化铝膜覆盖在 HZSM-5 分子筛的颗粒外层. 所制备的催化剂都具有较多的大孔和介孔比表面积, 在低温 (235 oC) 和高空速 (30 h–1) 条件下具有较高的甲醇脱水反应活性和稳定性, 其中在化学沉淀法制备的组合 Al2O3-HZSM-5 催化剂上, 二甲醚产率达到 13.5 g/(g•h).

Synthesis of Dimethyl Ether via Methanol Dehydration over Combined Al2O3-HZSM-5 Solid Acids

Combined Al2O3-HZSM-5 solid acids were prepared and used for methanol dehydration to dimethyl ether (DME) in a fixed-bed reactor. The physicochemical properties of the combined solid acids were characterized by X-ray diffraction, field emission scanning electron microscopy, N2 adsorption, and NH3 temperature-programmed desorption. Al2O3 was highly dispersed in Al2O3-HZSM-5 after impregnation (Al2O3-HZSM-5-IM), while a layered Al2O3-covered HZSM-5 structure solid acid was synthesized via chemical precipitation (Al2O3-HZSM-5-CP). Both the combined Al2O3-HZSM-5 solid acids prepared by impregnation and chemical precipitation have a higher surface area and more meso- and macropores. The combined Al2O3-HZSM-5 solid acids exhibit higher methanol dehydration activity than pure Al2O3 and it possesses higher stability than pure HZSM-5 at a lower temperature (235 ?C) and a higher LHSV (30 h?1). The stable DME productivities for Al2O3-HZSM-5-IM and Al2O3-HZSM-5-CP at 235 ?C reached 12.7 and 13.5 g/(g•h), respectively.