In Crystallo Snapshots of Rh2-Catalyzed C–H Amination,Journal of the American Chemical Society

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In Crystallo Snapshots of Rh2-Catalyzed C–H Amination
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-12 , DOI: 10.1021/jacs.0c09842
Anuvab Das ₁ , Chen-Hao Wang ₁ , Gerard P. Van Trieste ₁ , Cheng-Jun Sun ₂ , Yu-Sheng Chen ₃ , Joseph H. Reibenspies ₁ , David C. Powers ₁

Affiliation

While X-ray crystallography routinely provides structural characterization of kinetically stable pre-catalysts and intermediates, elucidation of the structures of transient reactive intermediates, which are intimately engaged in bond-breaking and -making during catalysis, is generally not possible. Here, we demonstrate in crystallo synthesis of Rh2 nitrenoids that participate in catalytic C-H amination, and we characterize these transient intermediates as triplet adducts of Rh2. Further, we observe the impact of coordinating substrate, which is present in excess during catalysis, on the structure of transient Rh2 nitrenoids. By providing structural characterization of authentic C-H functionalization intermediates, and not kinetically stabilized model complexes, these experiments provide the opportunity to define critical structure-activity relationships.

中文翻译：

在 Rh2 催化的 C–H 胺化的晶体快照中

虽然 X 射线晶体学通常提供动力学稳定的前催化剂和中间体的结构表征，但通常不可能阐明瞬态反应中间体的结构，这些中间体与催化过程中的键断裂和形成密切相关。在这里，我们展示了参与催化 CH 胺化的 Rh2 氮烯类化合物的晶体合成，并且我们将这些瞬态中间体表征为 Rh2 的三线态加合物。此外，我们观察了在催化过程中过量存在的配位底物对瞬态 Rh2 氮烯化合物结构的影响。通过提供真实的 CH 官能化中间体的结构表征，而不是动力学稳定的模型复合物，

更新日期：2020-11-12

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