Carbon-nitrogen moieties are found in a wide range of compounds, ranging from bulk materials to fine chemicals, such as biological and pharmaceutical ingredients. More sustainable and efficient methods for constructing C-N bonds are desired and cross-dehydrogenative amination has emerged as an environmentally friendly and selective approach to fulfill this need. However, the potential of heterogeneous catalysis remains largely unexplored in this area. In this work, we investigate a straightforward strategy to immobilize FeCl on the linkers of a metal–organic framework (i.e. CAU-27-BIPY), which is capable of performing the direct C-N coupling of benzimidazole and THF using -butylhydroperoxide (TBHP) with an excellent yield of 92 % under mild reaction conditions. The versatility and applicability of this approach are demonstrated by successfully coupling a wide variety of -heterocycles and ethers, including for the synthesis of key pharmaceutical precursors. Furthermore, the Fe-loaded MOF catalyst preserves its activity and structure over four consecutive runs.

中文翻译：

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负载铁的金属有机骨架 (CAU-27-Fe) 作为有效的多相催化剂，用于使用 NH 杂环对醚进行直接 C-H 胺化


碳-氮部分存在于多种化合物中，从散装材料到精细化学品，例如生物和药物成分。人们需要更可持续、更有效的方法来构建 C-N 键，交叉脱氢胺化已成为满足这一需求的一种环境友好且选择性的方法。然而，多相催化的潜力在该领域仍未得到充分开发。在这项工作中，我们研究了一种将 FeCl 固定在金属有机框架（即 CAU-27-BIPY）的连接体上的简单策略，该策略能够使用 丁基过氧化氢 (TBHP) 进行苯并咪唑和 THF 的直接 C-N 偶联在温和的反应条件下，收率高达 92%。该方法的多功能性和适用性通过成功偶联各种杂环和醚得到证明，包括用于关键药物前体的合成。此外，载铁 MOF 催化剂在连续四次运行中仍保持其活性和结构。