Reactions of a geminal Sc/P Lewis pair with pyridotetrazole and beyond†

IF 3.3 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Dalton Transactions Pub Date : 2024-11-06 DOI:10.1039/D4DT02838D

Yiwen Guan, Xian Xu and Xin Xu

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Abstract

Frustrated Lewis pair (FLP) chemistry has undergone remarkable growth, among which rare-earth metal-based Lewis pairs have exhibited unique reactivity in recent years. Herein, treatment of the intramolecular Sc/P Lewis pair, i.e., (ArO)₂ScN(^tBu)PPh₂ (1, Ar = 2,6-^tBu₂-C₆H₃), with pyridotetrazole resulted in the formation of an FLP nitrene adduct with N₂ elimination, offering additional insights into the mechanism of transition-metal-catalyzed denitrogenative annulation of pyridotetrazole. Reactions of complex 1 with 1,3,5-triazine and benzo[c]cinnoline generated FLP-type products via Sc/P 1,2-addition to the CN bond and the NN bond, respectively. Furthermore, treatments of 1 with phenylacetylene, diazo, and azide compounds were also investigated, leading to the formation of a variety of metallacyclic complexes displaying typical FLP behaviors.

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双子座 Sc/P 刘易斯对与吡啶四氮唑及其他的反应

受挫路易斯对（FLP）化学经历了显著的发展，其中以稀土金属为基础的路易斯对近年来表现出独特的反应活性。在本文中，分子内 Sc/P Lewis 对（即 (ArO)2ScN(tBu)PPh2 (1, Ar = 2,6-tBu2-C6H3)）与吡啶四氮唑处理后，形成了具有 N2 消去作用的 FLP 芘加合物，为过渡金属催化吡啶四氮唑的脱氮环化机制提供了更多的见解。复合物 1 与 1,3,5-三嗪和苯并[c]噌啉的反应分别通过 C=N 键和 N=N 键的 Sc/P 1,2 加成生成了 FLP 型产物。此外，还研究了 1 与苯乙炔、重氮和叠氮化合物的处理，结果形成了多种具有典型 FLP 行为的金属环配合物。

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.