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When activated with fluorinated borate cocatalysts the trimetallic complexes [Cp*LnMe2]3 (Ln=Y, Lu; Cp*=C5Me5) promote efficiently the formation of high‐cis polybutadiene. Respective polyisoprenes instead bear much less pronounced microstructures, but reveal crosslinked products at lower polymerization temperatures. Varying the amount of cocatalyst, the emerging active species were examined by NMR...
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