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作 者:陈绪川 董梅[1] 牛宪军[1,2] 王凯[1,2] 陈刚[1,2] 樊卫斌[1] 王建国[1] 秦张峰[1]
机构地区:[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]中国科学院大学,北京100049
出 处:《催化学报》2015年第6期880-888,共9页
基 金:supported by the National Basic Research Program of China(973 Program,2011CB201400);the National Natural Science Foundation of China(21273263,21273264,21227002);the Natural Science Foundation of Shanxi Province of China(2012011005-2,2013021007-3)~~
摘 要: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.
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