Full Paper
Macromolecular
Reaction Engineering
wileyonlinelibrary.com (1 of 21) 1600044 © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim DOI: 10.1002/mren.201600044
The polymerization of ethylene is investigated in a semibatch solution reactor using
bis(n-propylcyclopentadienyl)hafnium dichloride catalyst and tetrakis(pentafluorophenyl)
borate dimethylanilinium salt ([B(C
6
F
5
)
4
]
-
[Me
2
NHPh]
+
) as the catalytic system. Trioctylalu-
minum (TOA) is used as impurity scavenger and alkylating agent. Ethylene pressure, poly-
merization temperature, TOA, borate, and catalyst concentrations are changed to investigate
ethylene polymerization kinetics with this catalyst system. A 2
3
central composite design,
augmented with extra runs to further explore the effect of some factors, is used as the sta-
tistical basis for the polymerization study. Ethylene propagation follows first-order kinetics.
Chain transfer to monomer, β-hydride elimination, and
transfer to TOA are the main chain transfer reactions. In addi-
tion to alkylating the catalyst precursor, TOA also deactivates
the catalyst. The mode of reactor addition for catalyst, borate,
and TOA has also been studied. When TOA and borate are
added sequentially to the reactor, followed by the catalyst,
the polymerization activity is lower than when the catalyst
and borate are added simultaneously, suggesting that compl-
exation with borate avoids deactivation reactions with TOA.
Ethylene Polymerization with a Hafnocene
Dichloride Catalyst Using Trioctyl Aluminum
and Borate: Polymerization Kinetics and
Polymer Characterization
Saeid Mehdiabadi, João B. P. Soares,* Jeffrey Brinen
Dr. S. Mehdiabadi, Prof. J. B. P. Soares
Department of Chemical and Materials Engineering
University of Alberta
Edmonton, Alberta, Canada
E-mail: jsoares@ualberta.ca
Dr. J. Brinen
Baytown Technology and Engineering Complex
ExxonMobil Chemical Company
Baytown, TX 77522, USA
1. Introduction
Metallocene catalysts are as old as Ziegler–Natta cata-
lysts. They were used in 1957 by Breslow and Newburg
to polymerize ethylene with bis(cyclopentdienyl)tita-
nium dichloride and diethylaluminum chloride.
[1]
The
catalytic system had low activity, similarly to Natta
and co-workers observations on a complex prepared
with triethylaluminum. This catalytic system did not
attract commercial interest because of its low poly-
merization activity. Efforts to polymerize olefins using
bis(cyclopentadienyl)zirconium complexes were also
unsuccessful, and the catalytic system was described
to be totally inactive. The field remained dormant until
1976 when Kaminsky and Sinn showed that adding a
small amount of water to trimethylaluminum (TMA)
before polymerizations with metallocenes could drasti-
cally enhance activity by a factor of 10 000 or more.
[2,3]
This led to the discovery of the highly efficient activator
methylaluminoxane (MAO), and revolutionized the field
of olefin polymerization with molecular catalysts. Since
then, polymerizations using metallocene complexes
became one of the hottest areas of research in the poly-
olefin field.
[4,5]
Macromol. React. Eng. 2017, , 1600044