Computational design of molecular homogeneous organometallic catalysts followed by experimental realization remains a significant challenge. Here, we report the development and use of a density functional theory transition-state model that provided quantitative prediction of molecular Cr catalysts for controllable selective ethylene trimerization and tetramerization. This computational model identified a general class of phosphine monocyclic imine (P,N)-ligand Cr catalysts where changes in the ligand structure control 1-hexene versus 1-octene selectivity. Experimental ligand and catalyst synthesis as well as reaction testing quantitatively confirmed predictions.

中文翻译：

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计算过渡态设计为控制乙烯三聚和四聚提供了经实验验证的Cr（P，N）催化剂

分子均相有机金属催化剂的计算设计以及随后的实验实现仍然是一个重大挑战。在这里，我们报告密度泛函理论过渡态模型的发展和使用，该模型为可控的选择性乙烯三聚和四聚提供了分子Cr催化剂的定量预测。该计算模型确定了一般类别的膦单环亚胺（P，N）-配体Cr催化剂，其中配体结构的变化控制着1-己烯对1-辛烯的选择性。实验性配体和催化剂的合成以及反应测试定量地证实了预测。