金瑞,张娜,陈娜,折浪,王雪艳,张鹏,王俊.化学通报,2022,85(9):1127-1132.
吡啶-2-甲醛共价接枝UiO-66-NH2负载铁系催化剂的合成及催化乙烯齐聚性能
Synthesis and Catalytic Performance in Ethylene Oligomerization of Pyridine-2-formaldehyde covalently grafted to UIO-66-NH2 supported iron catalyst
投稿时间:2021-10-30  修订日期:2022-01-16
DOI:
中文关键词:  金属有机骨架  后合成修饰法,铁系催化剂  乙烯齐聚
英文关键词:metal organic frameworks, post synthetic modification, iron catalyst, ethylene oligomerization
基金项目:黑龙江省大学生创新创业训练计划项目(202110220027)和黑龙江省博士后基金项目(16190016)资助
作者单位E-mail
金瑞 东北石油大学 166768047@qq.com 
张娜 东北石油大学 zhangna091685@163.com 
陈娜 长庆油田公司第一采油厂  
折浪 东北石油大学  
王雪艳 东北石油大学  
张鹏 东北石油大学  
王俊 东北石油大学  
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中文摘要:
      以金属有机骨架UiO-66-NH2和吡啶-2-甲醛为原料,经后合成修饰法,合成出吡啶-2-甲醛共价接枝UiO-66-NH2配体,然后利用吡啶-2-甲醛作为桥联基将FeCl2负载到UiO-66-NH2上,制备出一种新型吡啶-2-甲醛共价接枝UiO-66-NH2负载铁系催化剂。傅里叶红外变换光谱(FT-IR)、X射线衍射(XRD)、扫描电子显微镜(SEM)、电感耦合等离子体质谱(ICP)和氮气吸附-脱附等分析方法证实合成出产物的结构与理论设计的结构相符。在合成与表征的基础上,对其催化乙烯齐聚性能进行研究。实验结果表明,随反应温度和Al/Fe摩尔比升高,催化活性先升高后降低,丁烯选择性升高;随乙烯压力增加,催化活性持续升高,丁烯选择性降低。最佳反应条件下,该催化剂的活性可达6.43×104 g·(mol Fe·h)-1,丁烯的选择性高达91.01%以上。
英文摘要:
      Pyridine-2-formaldehyde covalently grafted to UIO-66-NH2 ligand was prepared by post synthetic modification with metal organic frameworks (MOFs) UiO-66-NH2 and pyridine-2-formaldehyde as raw materials, and then a novel pyridine-2-formaldehyde covalently grafted to UIO-66-NH2 supported iron catalyst was synthesized by using pyridine-2-formaldehyde as bridging group to load FeCl2 onto UIO-66-NH2. The fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscope, inductively coupled plasma mass spectrometry and nitrogen adsorption-desorption confirmed that the structures of the synthesized products were consistent with the theoretical design structures. On the basis of synthesis and characterization, the catalytic oligomerization of ethylene was studied. The results show that with the increase of reaction temperature and Al/Fe mole ratio, the catalytic activity increased at first and then decreased, and the selectivity of butene increased.?With the increase of ethylene pressure, the catalytic activity increasd, but the selectivity of butene decreased. The catalytic activity of 6.43×104 g·(mol Fe·h)-1 and 91.01% selectivity of butene were obtained under the optimal reaction conditions.
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