Facile Synthesis of Rh Anchored Uniform Spherical COF for One-Pot Tandem Reductive Amination of Aldehydes to Secondary Imines,ACS Applied Materials & Interfaces

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Facile Synthesis of Rh Anchored Uniform Spherical COF for One-Pot Tandem Reductive Amination of Aldehydes to Secondary Imines
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-05-19 , DOI: 10.1021/acsami.1c05732
Nan Wang _{1,

2} , Jianguo Liu _{2,

3} , Long Tang ₂ , Xiuzhi Wei _{2,

4} , Chenguang Wang ₂ , Xinjun Li ₂ , Longlong Ma _{1,

2}

Affiliation

The development of transition metal-based heterogeneous catalysts for economical and efficient synthesis of secondary imines remains both desirable and challenging. Herein, for the first time, we present two kinds of Rh nanoparticle anchored uniform spherical COF heterogeneous catalysts with well-defined crystalline structures for the effective one-pot tandem reductive amination of aldehydes on a gram scale. This reaction is carried out using ammonia as a nitrogen source and hydrogen gas as the source of hydrogen, which is not only an atom-economical but also an environmentally friendly process for the selective production of secondary imines. In particular, in the presence of the better-designed Rh nanoparticles anchored COF2 catalyst, the starting material aldehydes could be fully converted (99% conversion), and 95% selectivity of N-benzylidene(phenyl)methanamine is obtained under mild reaction conditions (2 MPa of H₂ and 90 °C). Additionally, the Rh/COF2 catalyst is also applied to a variety of substituted aromatic aldehyde compounds, manifesting good yields in corresponding secondary imines. This work not only expands the COF family but also offers economical and effective access to acquire various aromatic amine targets, especially secondary imines.

中文翻译：

用于醛一锅串联还原胺化成仲亚胺的 Rh 锚定均匀球形 COF 的简便合成

用于经济有效合成仲亚胺的过渡金属基多相催化剂的开发仍然是可取的和具有挑战性的。在此，我们首次提出了两种具有明确晶体结构的 Rh 纳米颗粒锚定的均匀球形 COF 多相催化剂，用于在克级有效地一锅串联还原胺化醛。该反应以氨为氮源，氢气为氢源，是一种原子经济且环境友好的选择性生产仲亚胺的工艺。特别是，在设计更好的 Rh 纳米粒子锚定 COF2 催化剂的存在下，原料醛可以完全转化（99% 转化率），95% 的选择性N-亚苄基(苯基)甲胺在温和的反应条件(2 MPa的H ₂和90°C)下获得。此外，Rh/COF2 催化剂还应用于多种取代的芳香醛化合物，在相应的仲亚胺中表现出良好的收率。这项工作不仅扩展了 COF 家族，而且还提供了经济有效的途径来获得各种芳香胺目标，尤其是仲亚胺。

更新日期：2021-06-02

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