| 张娜,李昱颖,唐静,唐健杰,王俊.化学通报,2021,84(5):474-479. |
| MixMOFs接枝PNP铬系催化剂的合成及催化乙烯齐聚性能 |
| Synthesis and Catalytic Performance in Ethylene Oligomerization of Mixture Metal Organic Frameworks Graft PNP Chromium Catalyst |
| 投稿时间：2020-10-16 修订日期：2021-01-20 |
| DOI： |
| 中文关键词: 混合金属有机骨架 铬系催化剂 乙烯齐聚 催化性能 |
| 英文关键词:Mixture metal organic frameworks Chromium catalyst Ethylene oligomerization Catalytic property |
| 基金项目:黑龙江省博士后科学基金项目（16190016）和东北石油大学青年科学基金项目（2018QNL-13）资助 |
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| 中文摘要: |
| 以对苯二甲酸、2-氨基对苯二甲酸和六水合硝酸锌为原料，合成出一种含有氨基的混合金属有机骨架（MixMOFs），然后以MixMOFs、氯代二苯基磷和CrCl3（THF）3为原料，依次经后合成修饰法和络合反应，合成出一种新型的MixMOFs接枝PNP铬系催化剂。利用红外光谱、X-射线衍射、扫描电镜、元素分析和电感耦合等离子体质谱等方法对产物的结构进行表征，并考察了催化体系和反应条件对催化乙烯齐聚性能的影响。结果表明，MixMOFs接枝PNP铬系催化剂具有较好的催化乙烯齐聚性能，以环己烷为溶剂、一氯二乙基铝（Et2AlCl）为助催化剂，当反应温度为25℃、Al/Cr摩尔比为600、乙烯压力为1.0MPa时，该催化剂的活性可达4.33×104g/（mol Cr·h），聚合产物主要是C8以下的低碳烯烃，含量高达90%以上。并且催化剂重复使用3次，活性和选择性没有明显变化，表现出较好的重复利用性。 |
| 英文摘要: |
| Mixture metal organic frameworks (MixMOFs) was synthesized with terephthalic acid, 2-amino-terephthalic acid and zinc nitrate hexahydrate as starting materials. Then a novel MixMOFs graft PNP chromium catalyst was synthesized by post synthetic modification and complexation with MixMOFs, chlorodiphenylphosphine and CrCl3(THF)3 as raw materials. The structure of the MixMOFs graft PNP chromium catalyst was characterized by FTIR, XRD, SEM, elemental analysis and ICP. The effects of catalytic system and reaction conditions on catalytic performance in ethylene oligomerization were investigated. The results showed that the catalyst exhibits better catalytic performance in ethylene oligomerization. When cyclohexane is used as solvent and Et2 AlCl is used as co-catalyst, the catalytic activity of 4.33×104g/(mol Cr·h) and more than 90% selectivity of less than C8 olefins are obtained under the condition of the reaction temperature 25℃, Al/Cr molar ratio 600 and ethylene pressure 1.0 MPa. Moreover, the activity and selectivity did not change significantly after reused three times, showing good reusability. |
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