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作 者:任文超[1] 华子乐[1] 葛同广 周晓霞[1] 陈立松[1] 朱颜[1] 施剑林[1]
机构地区:[1]中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室,上海200050
出 处:《催化学报》2015年第6期906-912,共7页
基 金:supported by the National Basic Research Program of China(2013CB933200);the High Technology Research and Development Program of China(2012AA062703);China National Funds for Distinguished Young Scientists(51225202);the Opening Projects of State Key Laboratory of Heavy Oil Processing(SKLOP201402003)~~
摘 要:基于脱铝多级孔BEA沸石与二氯二茂钛的固相反应,开展了钛掺杂量可调的多级孔Ti-beta后处理工艺制备研究.对制备的多级孔Ti-beta样品的理化性质进行了表征,包括X射线衍射、氮气吸附脱附测试、扫描电镜、透射电镜、紫外可见吸收光谱和紫外拉曼光谱等.结果表明,多级孔BEA沸石具有较好的化学稳定性,脱铝-钛化的后处理过程未对样品多级孔结构产生明显影响.以环己烯和十二烯的烯烃环氧化为探针反应表征了合成多级孔Ti-beta与纯相微孔Ti-beta沸石的催化性能.结果表明,在小分子环己烯的环氧化反应中,多级孔Ti-beta沸石的催化活性(转化率59.4%)与微孔Ti-beta相当(转化率57.9%);但是在较大分子十二烯的催化反应中,多级孔结构Ti-beta材料的催化性能(转化率11.1%)明显优于纯相微孔材料(转化率6.8%),且产物中环氧化物选择性更高(分别为60.3%和37.8%).Hierarchically structured Ti-β zeolites were prepared using a two-step post-synthesis approach. The physicochemical properties of the resultant Ti-mβ-Sx materials were determined using various techniques, including X-ray diffraction, scanning electron microscopy, inductively coupled plasma atomic emission spectroscopy, transmission electron microscopy, and ultraviolet-visible and ultra-violet-Raman spectroscopies. The porous structures of the synthesized hierarchical Ti-β zeolites were well preserved. Their catalytic performance was compared with that of pure microporous Ti-βmaterials using alkene epoxidation as a model reaction. It was found that although comparable catalytic activities were obtained for both types of catalyst in the epoxidation of small molecules, e.g., cyclohexene, the synthesized hierarchical Ti-βgave an enhanced catalytic performance in the epoxidation of bulky 1-dodecene.
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