期刊
POLYMERS
卷 11, 期 7, 页码 -出版社
MDPI
DOI: 10.3390/polym11071114
关键词
tandem catalysis; in-situ copolymerization; linear low-density polyethylene; non-metallocene; binuclear titanium complex
资金
- National Natural Science Foundation of China [21172269]
- Key Laboratory of Optoelectronic Chemical Materials and Devices, Ministry of Education, Jianghan University [JDGD-201809]
- Hubei Provincial Department of Education [B2017270]
A novel tandem catalysis system consisted of salicylaldiminato binuclear/mononuclear titanium and 2,6-bis(imino) pyridyl iron complexes was developed to catalyze ethylene in-situ copolymerization. Linear low-density polyethylene (LLDPE) with varying molecular weight and branching degree was successfully prepared with ethylene as the sole monomer feed. The polymerization conditions, including the reaction temperature, the Fi/Ti molar ratio, and the structures of bi-or mononuclear Ti complexes were found to greatly influence the catalytic performances and the properties of obtained polymers. The polymers were characterized by differential scanning calorimetry (DSC), high temperature gel permeation chromatography (GPC) and high temperature C-13 NMR spectroscopy, and found to contain ethyl, butyl, as well as some longer branches. The binuclear titanium complexes demonstrated excellent catalytic activity (up to 8.95 x 10(6) g/molTi.h.atm) and showed a strong positive comonomer effect when combined with the bisiminopyridyl Fe complex. The branching degree can be tuned from 2.53 to 22.89/1000C by changing the reaction conditions or using different copolymerization pre-catalysts. The melting points, crystallinity and molecular weights of the products can also be modified accordingly. The binuclear complex (TiL1)-L-2 with methylthio sidearm showed higher capability for comonomer incorporation and produced polymers with higher branching degree and much higher molecular weight compared with the mononuclear analogue.
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