122
ISSN 1560-0904, Polymer Science, Series B, 2018, Vol. 60, No. 1, pp. 122–129. © Pleiades Publishing, Ltd., 2018.
Ethylene/1-Hexene Copolymerization and Synthesis
of LLDPE/Nanocarbon Composite through In Situ Polymerization
1, 2
Nikoo Nabizadeh
a
, Gholam Hossein Zohuri
a,
*, Mostafa Khoshsefat
b
,
Navid Ramezanian
a
, and Saeid Ahmadjo
b
a
Department of Chemistry, Faculty of Science, Ferdowsi University of Mashhad, Mashhad, Iran
b
Department of Catalyst, Iran Polymer and Petrochemical Institute, Tehran, Iran
*e-mail: zohuri@um.ac.ir
Received April 7, 2017;
Revised Manuscript Received July 21, 2017
Abstract—Copolymerization of ethylene/1-hexene using a modified ZN-type catalyst was carried out in the
presence of triethylaluminium as cocatalyst. The optimum copolymerization activity was obtained at Al : Ti =
357 : 1, 60°C and the comonomer concentration of 0.6 mol/L in the range studied. Copolymer/nanocarbon
(including multiwalled carbon nanotube, graphene nanoplatelet) composites were prepared via in-situ
polymerization. The copolymerization activity decreased by addition of the nanocarbon into the reactor. The
presence of graphene nanoplatelet in nanocomposites reduced the melting temperature and increased heat of
fusion, crystallinity and density of the obtained polymer. In the copolymer/carbon nanotube nanocompos-
ites, decreasing of melting temperature was observed in comparison to pure copolymer, whereas, heat of
fusion, crystallinity and density increased. The results of TGA analysis showed that the addition of nanocar-
bons has improved the thermal stability of obtained copolymers.
DOI: 10.1134/S1560090418010104
INTRODUCTION
Nowadays, polyolefins play an important role in
many applications, particularly linear low-density
polyethylene (LLDPE). LLDPE is very attractive
polymer due to its excellent properties, such as low
density, good mechanical properties, easy fabrication
and recycling [1–3]. LLDPE is a copolymer of eth-
ylene with C
4
–C
8
α-olefins. Because it contains a
small amount of short-chain branches along the back-
bone of polymer chains, the crystallinity, melting tem-
perature, and density are lower than for ethylene
homopolymer. Introduction of α-olefin comonomer
into the polyethylene chain alters the structure, and
consequently the properties of the polymer product
obtained. This effect is dependent on the type of cata-
lytic system used, polymerization conditions as well as
the comonomer type that is introduced [4–8].
Among all of PE grades, the LLDPE offers many
interesting properties; however, its relatively low creep
resistance, barrier of oxygen, poor stiffness and elec-
trical conductivity may limit its application in some
fields. Based on this, addition of small amounts of
nanoparticles have proved to play a beneficial role in
1
The article is published in the original.
2
Supplementary materials are available for this article at
10.1134/S1560090418010104 and are accessible for authorized
users.
improving of its applications in packaging, electronics
industries, etc. [9–14].
Synthesis of nanocomposites can be carried out by
three main methods; in situ polymerization, solution
and melt mixing [14–19]. Among these methods, in
situ polymerization is one of the most promising and
efficient methods to synthesize polyolefin nanocom-
posites [14]. The nanocarbons such as carbon nano-
tube, graphene nanoplatelets, etc. with their striking
features of the polymer properties have captured
attention of numerous researchers. For instance,
Kaminsky et al. used multi-walled carbon nanotubes
(CNTs) through in situ polymerization method for
ethylene and propylene homopolymerization. Activi-
ties of single site metallocene catalysts decreased as the
percentage of nanotubes increased. They also
observed increasing in crystallization temperature and
variations in molecular weight polyethylene and poly-
propylene composites. Moreover, the presence of
CNTs in polymer matrices resulted in a significant
improvement in electrical conductivity as well as
improved mechanical strength [20]. Boggioni synthe-
sized ethylene-co-norbornene copolymers grafted
CNTs composites by in situ polymerization in the
presence of Ti-based catalyst and MAO as co-catalyst.
Based on the results, the grafted CNTs caused increas-
ing in glass transition temperature and Young’s mod-
ulus in comparison neat ethylene/norbornene copoly-
mer [21].
COMPOSITES