石油学报(石油加工)2024,Vol.40Issue(3) :637-649.DOI:10.3969/j.issn.1001-8719.2024.03.008

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 Over PAMAM Grafted Carbon Nanotubes Supported Nickel Catalyst

李杨 郭丽君 霍宏亮 黄金 蒋岩 李锋 李翠勤
石油学报(石油加工)2024,Vol.40Issue(3) :637-649.DOI:10.3969/j.issn.1001-8719.2024.03.008

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 Over PAMAM Grafted Carbon Nanotubes Supported Nickel Catalyst

李杨 1郭丽君 1霍宏亮 2黄金 1蒋岩 2李锋 1李翠勤1
扫码查看

作者信息

  • 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
  • 折叠

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.

Abstract

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-carbon α-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-carbon α-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

Key words

α-olefin/carbon nanotube/polyamide amine/dendritic nickel catalyst/ethylene oligomerization/grey correlation analysis

引用本文复制引用

基金项目

黑龙江省重点研发计划(JD22A026)

出版年

2024
石油学报(石油加工)
中国石油学会

石油学报(石油加工)

CSTPCD北大核心
影响因子:0.764
ISSN:1001-8719
参考文献量37
段落导航相关论文