PAMAM接枝碳纳米管负载镍催化剂高选择性制备低碳烯烃  

Highly Selective Preparation of Low Carbon Olefins OverPAMAM Grafted Carbon Nanotubes Supported Nickel Catalyst

作　　者：李杨[1] 郭丽君 霍宏亮 黄金[1] 蒋岩[2] 李锋[1] 李翠勤[1] LI Yang;GUO Lijun;HUO Hongliang;HUANG Jin;JIANG Yan;LI Feng;LI Cuiqin(Key Laboratory of New Polyolefin Materials,College of Chemistry and Chemical Engineering,Northeast Petroleum University,Daqing 163318,China;Daqing Petrochemical Research Center,PetroChina Company Limited,Daqing 163714,China)

机构地区：[1]东北石油大学化学化工学院聚烯烃新材料重点实验室,黑龙江大庆163318 [2]中国石油天然气股份有限公司大庆化工研究中心,黑龙江大庆163714

出　　处：《石油学报（石油加工）》2024年第3期637-649,共13页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：黑龙江省重点研发计划项目(JD22A026)基金资助。

摘　　要：成功合成聚酰胺-胺型(PAMAM)树枝状镍催化剂(PAMAM-Cat)和PAMAM功能化接枝碳纳米管负载镍催化剂(CNT-PAMAM-Cat)。采用傅里叶变换红外光谱、X射线衍射、光电子能谱等手段对2种催化剂进行表征,系统考察温度、助催化剂用量、压力、时间对其催化乙烯齐聚制备低碳α-烯烃的影响。结果表明:在最佳聚合条件(温度25℃、Al/Ni摩尔比500(PAMAM-Cat)和700(CNT-PAMAM-Cat)、压力0.7 MPa、时间0.5 h)下,2种催化剂表现出优异的乙烯齐聚反应活性(5.75×104和3.75×104 g/(mol Ni·h))和低碳α-烯烃选择性,CNT-PAMAM-Cat催化剂经过3次重复实验后的反应活性不变;基于灰色关联分析得出,压力是影响2种催化剂催化乙烯齐聚生成低碳α-烯烃的关键因素。Polyamide amine(PAMAM)dendritic nickel catalyst(PAMAM-Cat)and PMAMA functionalized grafted carbon nanotubes supported nickel catalyst(CNT-PAMAM-Cat)were successfully synthesized,and these two catalysts were characterized by Fourier transforms infrared spectroscopy,X-ray diffraction and photoelectron spectroscopy.Moreover,the effects of temperature,co-catalyst dosage,pressure,and time on the preparation of low-carbonα-olefins by catalytic ethylene oligomerization were also systematically investigated.The results indicate that under the optimal polymerization conditions(temperature 25℃,Al/Ni molar ratio 500(PAMAM-Cat)and 700(CNT-PAMAM-Cat),pressure 0.7 MPa,time 0.5 h),the two catalysts exhibit excellent ethylene oligomerization activities(5.75×104 and 3.75×104 g/(mol Ni·h))and low-carbonα-olefin selectivity.After three times of reutilization,CNT-PAMAM-Cat activity remains unchanged.The grey correlation analysis shows that pressure is a key factor affecting ethylene oligomerization over the two catalysts to produce low-carbonα-olefins.

关 键 词：Α-烯烃 碳纳米管 聚酰胺 树枝状镍催化剂 乙烯齐聚 灰色关联分析 

分 类 号：O643.3[理学—物理化学]