摘要
合成了一种N,N-二齿配位的新型树枝状桥联吡啶亚胺配体及其镍配合物,利用元素分析、傅里叶变换红外光谱（FTIR）和电喷雾电离质谱（ESI-MS）对其结构进行了表征.以二氯乙基铝（Et Al Cl2）为助催化剂,考察了树枝状桥联镍配合物催化乙烯齐聚和1-戊烯齐聚的聚合条件对产物分布的影响.结果表明,当聚合时间为60 min,聚合压力为0.5 MPa,Al/Ni摩尔比为150时,乙烯齐聚产物中C10~C14的选择性最高,达到93%,催化活性为0.99×106g/（mol Ni·h）;当聚合时间为60 min,Al/Ni摩尔比为300时,1-戊烯齐聚产物中C20的选择性最高为70.5%,催化活性为2.47×105g/（mol Ni·h）.该树枝状桥联镍配合物对乙烯齐聚反应和1-戊烯齐聚反应均具有良好的催化活性和较高碳数的齐聚产物选择性.
A novel N,N-bidentate dendritic bridging pyridine-imine ligand and its nickel complex were prepared and characterized by elemental analysis, Fourier transform infrared spectrometry（ FTIR） and electrospray ionization-mass spectrometry（ ESI-MS）. The dendritic nickel complex was used as a precatalyst in the oligomerization of ethylene with the co-catalyst ethyl dichloroaluminum（ Et Al Cl2）,as well as a precursor in the oligomerization of 1-pentene. The effects of the reaction time,reaction pressure and the molar ratio of Al / Ni on the catalytic activities and the distribution of the product in the oligomerization were investigated.The dendritic nickel complex revealed the selectivity of higher olefins（ C10—C14） reached up to 93% and the catalytic activity was 0. 99 × 106 g /（ mol Ni·h） at the reaction time of 60 min,ethylene pressure of 0. 5 MPa and the molar ratio of Al / Ni of 150 in the oligometization of ethylene. At the reaction time of 60 min and the molar ratio of Al / Ni of 300,the catalyst also had excellent catalytic performance in the oligomerization of1-pentene. The selectivity of C20 reached to 70. 5% and the catalytic activity was 2. 47 × 105 g /（ mol Ni·h）.The dendritic nickel complex exhibited good catalytic activities and selectivities for higher carbon number olefins in ethylene oligomerization and 1-pentene oligomerization.
出处
《高等学校化学学报》
SCIE
EI
CAS
CSCD
北大核心
2015年第9期1813-1818,共6页
Chemical Journal of Chinese Universities
基金
国家自然科学基金(批准号:21576048)
中国石油科技创新基金研究项目(批准号:2014D-5006-0503)
东北石油大学青年科学基金(批准号:2013NQ130)资助~~
关键词
树枝状大分子
桥联镍配合物
乙烯齐聚
1-戊烯齐聚
Dendrimer
Bridging nickel complex
Ethylene oligomerization
1-Pentene oligomerization
