Combining Both Acceptorless Dehydrogenation and Borrowing Hydrogen Mechanisms in One System as Described by DFT Calculations,Advanced Theory and Simulations

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Combining Both Acceptorless Dehydrogenation and Borrowing Hydrogen Mechanisms in One System as Described by DFT Calculations
Advanced Theory and Simulations ( IF 2.9 ) Pub Date : 2022-04-12 , DOI: 10.1002/adts.202100566
Alessandra Cicolella _{1,

2} , Massimo C. D'Alterio _{1,

3} , Josep Duran ₁ , Sílvia Simon ₁ , Giovanni Talarico ₂ , Albert Poater ₁

Affiliation

The mechanisms for the formation of N-substituted hydrazones by coupling of alcohols and hydrazine, achieved by the sequential processes of acceptorless dehydrogenation and borrowing hydrogen, has been unveiled by density functional theory (DFT) calculations. The release of water and molecular hydrogen as subproducts, combined with the Mn-PNN pincer based catalyst describe a green environment. Mechanistically, apart from describing a complex system of three coupled catalytic pathways, calculations describe the pivotal role of two intermediates, which participate in two catalytic pathways each one. Finally, predictive catalysis plays the role to push forward this reaction toward milder conditions, and thus in line with green chemistry standards.

中文翻译：

如 DFT 计算所述，在一个系统中结合无受体脱氢和借氢机制

密度泛函理论 (DFT) 计算揭示了通过无受体脱氢和借氢的顺序过程实现的醇和肼偶联形成 N-取代腙的机制。作为副产物的水和分子氢的释放，与基于 Mn-PNN 钳形催化剂的结合描述了绿色环境。从机理上讲，除了描述三个耦合催化途径的复杂系统外，计算还描述了两个中间体的关键作用，它们各自参与两个催化途径。最后，预测催化作用可将这一反应推向更温和的条件，从而符合绿色化学标准。

更新日期：2022-04-12

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