朱志荣,谢在库,陈庆龄,杨为民,李为,李灿.ZSM-5表面酸性的CLD改性及其对择形催化性能的影响[J].分子催化,2007,(1):79-81 |
ZSM-5表面酸性的CLD改性及其对择形催化性能的影响 |
CLD Modification for Acidity of ZSM-5 and Its Effect on the Shape-Selective Catalysis |
修订日期:2006-12-05 |
DOI: |
中文关键词: 化学气相硅沉积 ZSM-5 择形催化 表面酸性 改性 |
英文关键词:CLD modification,shape-selectivity,acidity,catalysis,ZSM-5 |
基金项目: |
朱志荣 谢在库 陈庆龄 杨为民 李为 李灿 |
中国科学院大连化学物理研究所,辽宁,大连,116023;中石化上海石油化工研究院,上海,201208 中石化上海石油化工研究院,上海,201208 中石化上海石油化工研究院,上海,201208 中石化上海石油化工研究院,上海,201208 中石化上海石油化工研究院,上海,201208 中国科学院大连化学物理研究所,辽宁,大连,116023 |
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中文摘要: |
为了获得分子筛催化反应中所需产物的高择形催化选择性,往往必须消除分子筛外表面酸性和减少孔道开口尺寸.目前,各种改性方法已被用于提高ZSM-5的选择性,例如金属、非金属化合物的浸渍,化学气相硅沉积(SiO2-CVD)和预结焦处理等1.虽然采用大分子有机物可以消除分子筛外表面的酸性位,但这种改性在反应条件下尤其在高的反应温度下是不稳定的2.…… |
英文摘要: |
SiO2-CLD modification for ZSM-5 acidity was investigated by pyrolysis gas chromatography-mass spectrometer (PGC-MS), Py-IR, NH3-TPD. In SiO2-CLD modification, the decomposition of polysiloxane to silica is the acid-catalyzed degradation combing the thermal pyrolysis, with the following oxidation at high temperature. Though the silanol groups disappear after the modification, most of the framework bridging hydroxyls and non-framework-Al hydroxyls remain. Besides, the acidic amount of the modified ZSM-5 drops gradually with increasing extent of modification, but the acidic strength distribution of the modified ZSM-5 is similar to that of parent ZSM-5. After two-cycle modification, TIPB conversion of the modified ZSM-5 is reduced by 95%, so its external surface may be regarded to be nearly inactive. The activity for cracking of 1,3,5-triisopropylbenzene (TIPB) is close to zero over the modified ZSM-5, but the modified ZSM-5 retains high activity for cracking of cumene. So, SiO2-CLD with polysiloxane is an ideal way of modification for obtaining the shape-selective ZSM-5 catalyst. |
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