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Highly selective cross‐hydroalkenylations of endocyclic 1,3‐dienes at the least substituted site with α‐olefins were achieved with a set of neutral (NHC)NiIIH(OTf) catalysts and cationic NiII catalysts with a novel NHC ligand. Under heteroatom assistance, skipped dienes were obtained in good yields, often from equal amounts of the two substrates and at a catalyst loading of 2–5 mol %. Rare 4,3‐product...
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