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An unprecedented level of control for the radical polymerization of vinylidene fluoride (VDF), yielding well‐defined PVDF (at least up to 14 500 g mol−1) with low dispersity (≤1.32), was achieved using organometallic‐mediated radical polymerization (OMRP) with an organocobalt compound as initiator. The high chain‐end fidelity was demonstrated by the synthesis of PVDF‐ and PVAc‐containing di‐and triblock...
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