Abstract
Brookhart's nickel α-diimine complex [(κ2-N,N-BIAN)NiCl2] (1) (where BIAN = {Ar-NAceN-Ar}, Ace = acenaphthen-1,2-diyl, and Ar = 2,6-(iPr)2-C6H3) activated with a hydrosilane/B(C6F5)3 (SiHB) adduct forms a highly active catalytic system for ethylene polymerization. Under optimal conditions, the activity of the system depends on the nature of hydrosilane and decreases in the order R3SiH > Ph2SiH2 > PhSiH3. The decrease in system activity within the hydrosilane series is correlated with increasing formation of Ni(I) species. In addition to their activation effect, hydrosilanes act as efficient chain termination/chain transfer agents, with the Si/Ni ratio controlling the molecular weight of the resulting polyethylene (PE). The use of Et3SiH generated elastomeric, highly branched polymers with a saturated chain-end, while systems using Ph2SiH2 and PhSiH3 led to branched end-functionalized PEs terminated with the hydrosilyl functionality (i.e. br-PE-SiPh2H or br-PE-SiPhH2).
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