Ruthenium‐Catalyzed Secondary Amine Formation Studied by Density Functional Theory,ChemCatChem

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Ruthenium‐Catalyzed Secondary Amine Formation Studied by Density Functional Theory
ChemCatChem ( IF 3.8 ) Pub Date : 2020-11-25 , DOI: 10.1002/cctc.202001588
Lukas Hückmann ₁ , Sonia Álvarez‐Barcia ₁ , Marina Fuhrer _{2,

3} , Bernd Plietker _{2,

3} , Johannes Kästner ₁

Affiliation

Amines are a ubiquitous class of compounds found in a variety of functional organic building blocks. Within the past years, hydrogen autotransfer catalysis has evolved as a new concept for the synthesis of amines. A through understanding of the mechanism of these reactions is necessary to design optimal catalysts. We investigate secondary amine formation catalyzed by a NNNN(P)Ru‐complex and provide understanding on the three reaction steps involved. We find that the ligand has to open one coordination site in order to allow the formation of a metal hydride intermediate. In a second step, a condensation reaction, which could also happen uncatalyzed in solution, is significantly enhanced by the presence of the ruthenium complex. The back‐transfer of the hydride to the substrate in a third step regenerates the catalyst.

中文翻译：

密度泛函理论研究钌催化的仲胺形成

胺是在各种功能性有机构件中发现的一类普遍存在的化合物。在过去的几年中，氢自动转移催化已经发展成为合成胺的新概念。对这些反应机理的透彻理解对于设计最佳催化剂是必要的。我们研究了由NNNN（P）Ru络合物催化的仲胺形成，并提供了对涉及的三个反应步骤的理解。我们发现，配体必须打开一个配位位点以允许金属氢化物中间体的形成。在第二步骤中，钌络合物的存在显着增强了缩合反应，该缩合反应也可能在溶液中未催化发生。氢化物在第三步中向基材的逆转会再生催化剂。

更新日期：2020-11-25

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