Here we report the in situ generation of nucleophilic allylboranes from H₂ and allenes mediated by a pyridonate borane that displays frustrated‐Lewis‐pair reactivity. Experimental and computational mechanistic investigations reveal that upon H₂ activation, the covalently bound pyridonate substituent becomes a datively bound pyridone ligand. Dissociation of the formed pyridone borane complex liberates Piers borane and enables a hydroboration of the allene. The allylboranes generated in this way are reactive towards nitriles. A catalytic protocol for the formation of allylboranes from H₂ and allenes and the allylation of nitriles has been devised. This catalytic reaction is a conceptually new way to use molecular H₂ in organic synthesis.

中文翻译：

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由显示出沮丧的路易斯对反应性的吡啶酸酯硼烷催化的分子氢和丙二烯催化的亲核烯丙基硼烷的形成。

在这里，我们报道了由H ₂和丙二烯介导的亲核烯丙基硼烷原位生成，其表现出沮丧的刘易斯对反应性。实验和计算机制研究表明，在H ₂活化后，共价结合的吡啶酸酯取代基成为固定结合的吡啶酮配体。形成的吡啶酮硼烷络合物的离解释放了Piers硼烷，并使丙二烯进行硼氢化。以这种方式产生的烯丙基硼烷对腈具有反应性。已经设计了用于由H ₂和烯丙基形成烯丙基硼烷和腈的烯丙基化的催化方案。从概念上讲，这种催化反应是使用分子H _2的新方法 在有机合成中。