Zn物种对乙烯芳构化反应过程的影响（英文）

Influence of Zn species in HZSM-5 on ethylene aromatization

分别采用离子交换法和物理混合法制备了不同Zn含量的ZSM-5分子筛催化剂,采用X射线衍射、扫描电子显微镜、N2物理吸附、氨程序升温脱附、吡啶红外吸附光谱、紫外-可见光谱和X射线光电子能谱等技术研究了催化剂的结构、表面性质及Zn物种种类,探讨了Zn物种存在状态对乙烯芳构化反应的影响.结果表明,引入到HZSM-5中的Zn物种包括三种状态,即Zn O晶体、存在于分子筛孔道中的Zn O团簇以及Zn和分子筛质子酸中心通过固相反应生成的Zn(OH)+物种;不同的制备方法显著影响Zn物种的分布.比较了制备方法和Zn含量对ZSM-5分子筛催化剂在乙烯芳构化反应中性能的影响,发现Zn(OH)+物种是芳构化的主要活性中心,同时ZnO物种的存在有助于乙烯制芳烃反应的发生.

Zn-containing HZSM-5 zeolites with different Zn contents were prepared by ion exchange and physically mixing methods, and were characterized by X-ray diffraction, scanning electron micro-scope, N2 adsorption-desorption, NH3 temperature programmed desorption, pyridine adsorption infrared spectroscopy, ultraviolet-visible diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy. Zn species introduced into HZSM-5 were identified as ZnO crystals, ZnO clusters in the zeolite channel and Zn（OH）＋species formed from a solid state reaction between dispersed ZnO and the protons in the zeolite. The preparation method has a significant influence on the distribu-tion of the Zn species. The catalytic behavior of Zn-containing HZSM-5 with different Zn contents showed that the Zn（OH）＋and ZnO species were responsible for aromatic formation from ethylene.