An ideal synthesis of alkyl amines would involve the direct use of abundant and easily accessible molecules such as dinitrogen (N₂) and feedstock alkenes^1-4. However, this ambition remains a great challenge as it is usually difficult to simultaneously activate both N₂ and a simple alkene and combine them together through C‒N bond formation. Currently, the synthesis of alkyl amines relies on the use of ammonia produced via the Haber-Bosch process and prefunctionalised electrophilic carbon sources. Here we report the hydroamination of simple alkenes with N₂ in a trititanium hydride framework, which activates both alkenes and N₂, leading to selective C‒N bond formation and providing the corresponding alkyl amines on further hydrogenation and protonation. Computational studies reveal key mechanistic details of N₂ activation and selective C‒N bond formation. This work demonstrates a strategy for the transformation of N₂ and simple hydrocarbons into nitrogen-containing organic compounds mediated by a multinuclear hydride framework.

烷基胺的理想合成将涉及直接使用丰富且易于获得的分子，例如二氮 (N ₂ ) 和原料烯烃 ^1-4 。然而，这一目标仍然是一个巨大的挑战，因为通常很难同时激活 N ₂ 和简单的烯烃并通过 C-N 键形成将它们结合在一起。目前，烷基胺的合成依赖于使用通过哈伯-博世工艺生产的氨和预官能化的亲电子碳源。在这里，我们报道了简单烯烃与 N ₂ 在三钛氢化物框架中的氢胺化，这同时激活了烯烃和 N ₂ ，导致选择性 C-N 键形成并提供相应的烷基胺进一步氢化和质子化。计算研究揭示了 N ₂ 激活和选择性 C-N 键形成的关键机制细节。这项工作展示了一种通过多核氢化物框架介导的 N ₂ 和简单碳氢化合物转化为含氮有机化合物的策略。