Silica/MAO/(n-BuCp)2ZrCl2 catalyst: effect of support dehydroxylation temperature on the grafting of MAO and ethylene polymerization

被引:42
作者
Bashir, Muhammad Ahsan [1 ,3 ]
Vancompernolle, Tom [2 ]
Gauvin, Regis M. [2 ]
Delevoye, Laurent [2 ]
Merle, Nicolas [1 ]
Monteil, Vincent [1 ]
Taoufik, Mostafa [1 ]
McKenna, Timothy F. L. [1 ]
Boisson, Christophe [1 ]
机构
[1] Univ Lyon 1, CPE Lyon, CNRS, UMR 5265,C2P2, Bat 308F,43 Bd 11 Novembre 1918, F-69616 Villeurbanne, France
[2] Univ Lille Nord France, UCCS CNRS UMR 8181, USTL ENSCL, F-59652 Villeneuve Dascq, France
[3] Dutch Polymer Inst, POB 902, NL-5600 AX Eindhoven, Netherlands
关键词
SOLID-STATE NMR; GAS-PHASE; STRUCTURAL-CHARACTERIZATION; OLEFIN POLYMERIZATION; METALLOCENE CATALYSTS; ORGANOALUMINUM COMPOUNDS; ZIRCONOCENE CATALYSTS; TERT-BUTYLALUMINUM; ALUMINUM COMPLEXES; SILICA SURFACE;
D O I
10.1039/c5cy01285f
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The current study aims to explore the link between the role of silica dehydroxylation temperature and the catalytic performance of an (n-BuCp)(2)ZrCl2 metallocene precursor supported on silica impregnated with methylaluminoxane (MAO) in ethylene homopolymerization. Diffuse Reflectance Fourier Transform Infrared Spectroscopy (FT-IR-DRIFT) and Solid State Nuclear Magnetic Resonance (SS NMR) were used to study the generation of different Al species on the surface of silica impregnated with MAO after calcination at temperatures of 200 degrees, 450 degrees and 600 degrees C. It was found that Si-CH3 bonds can be formed when silica dehydroxylation temperature is >= 450 degrees C, and that three different types of aluminum species are generated on silica surface, the nature of which does not change significantly with the silica dehydroxylation temperature. After grafting a metallocene precursor on the MAO-treated surfaces, increases in the zirconium loading, and in the intrinsic and average catalytic activities were observed with increasing silica dehydroxylation temperature. However, the molecular and physical properties of the high density polyethylene produced by using these catalysts were observed to be independent of the silica dehydroxylation temperature. These results indicated that the number of active sites on the surface of the catalyst increased with increasing dehydroxylation temperature, but the nature of the active sites does not.
引用
收藏
页码:2962 / 2974
页数:13
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