School of Chemical Sciences, University of Illinois Urbana-Champaign, 600 S. Mathews Avenue, Urbana, IL 61801, USA.
School of Science, Technology, Engineering & Mathematics, University of Washington Bothell, Bothell, WA 98011, USA.
Sci Adv. 2023 Jun 9;9(23):eadg8130. doi: 10.1126/sciadv.adg8130.
The activation of inert C─H bonds by transition metals is of considerable industrial and academic interest, but important gaps remain in our understanding of this reaction. We report the first experimental determination of the structure of the simplest hydrocarbon, methane, when bound as a ligand to a homogenous transition metal species. We find that methane binds to the metal center in this system through a single M···H-C bridge; changes in the coupling constants indicate clearly that the structure of the methane ligand is significantly perturbed relative to the free molecule. These results are relevant to the development of better C─H functionalization catalysts.
过渡金属活化惰性 C─H 键具有重要的工业和学术意义，但我们对这一反应的理解仍存在重要的空白。我们报告了首例最简单的烃类甲烷作为均相过渡金属物种的配体时的结构的实验测定。我们发现甲烷在该体系中通过单个 M···H-C 桥与金属中心结合；耦合常数的变化清楚地表明，与游离分子相比，甲烷配体的结构受到了明显的干扰。这些结果与开发更好的 C─H 功能化催化剂有关。
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