Polyethylene is a highly apolar polymer with very poor
adhesion
to most substrates, necessitating the use of tie layers. Therefore,
the synthesis of functional polyethylene is a long-standing challenge
in catalytic ethylene polymerization. Here, we report the preparation
of a nanocomposite comprising polyethylene covalently grafted onto
sheet-like silsesquioxanes, with unprecedented adhesion to metal and
glass. A norbornene-grafted, layered Mg-silsesquioxane is treated
with Grubbs second-generation catalyst (G-II), and the identity of
covalently tethered G-II is unambiguously ascertained. Covalently
tethered G-II catalyzes the ring opening metathesis polymerization
of cyclooctene to poly(cyclooctene). The resulting poly(cyclooctene)
is catalytically hydrogenated to yield polyethylene. This polyethylene
nanocomposite exhibited a bonding strength of the order of 100 MPa
on stainless steel and aluminum, 10-fold higher than reported for
engineered polyethylene copolymers. The nanocomposite exhibits an
increase in the polar component of surface energy, yet remains compatible
and cocrystallizes with a polyethylene matrix.