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Uncovering the Activity of Alkaline Earth Metal Hydrogenation Catalysis Through Molecular Volcano Plots
Topics in Catalysis ( IF 3.6 ) Pub Date : 2021-08-25 , DOI: 10.1007/s11244-021-01480-7
Shubhajit Das 1 , Bart De Tobel 2 , Mercedes Alonso 2 , Clémence Corminboeuf 1
Affiliation  

Recent advances in alkaline earth (Ae) metal hydrogenation catalysis have broadened the spectrum of potential catalysts to include candidates from the main group, providing a sustainable alternative to the commonly used transition metals. Although Ae-amides have already been demonstrated to catalyze hydrogenation of imines and alkenes, a lucid understanding of how different metal/ligand combinations influence the catalytic activity is yet to be established. In this article, we use linear scaling relationships and molecular volcano plots to assess the potential of the Ae metal-based catalysts for the hydrogenation of alkenes. By analyzing combinations of eight metals (mono-, bi-, tri-, and tetravalent) and seven ligands, we delineate the impact of metal-ligand interplay on the hydrogenation activity. Our findings highlight that the catalytic activity is majorly determined by the charge and the size of the metal ions. While bivalent Ae metal cations delicately regulate the binding and the release of the reactants and the products, respectively, providing the right balance for this reaction, ligands play only a minor role in determining their catalytic activity. We show how volcano plots can be utilized for the rapid screening of prospective Ae catalysts to establish a guideline to achieve maximum activity in facilitating the hydrogenation process.



中文翻译:

通过分子火山图揭示碱土金属氢化催化的活性

碱土 (Ae) 金属加氢催化的最新进展拓宽了潜在催化剂的范围,包括来自主要族群的候选物,为常用的过渡金属提供了可持续的替代品。尽管已证明 Ae-酰胺可催化亚胺和烯烃的氢化,但尚未明确了解不同的金属/配体组合如何影响催化活性。在这篇文章中,我们使用线性比例关系和分子火山图来评估 Ae 金属基催化剂用于烯烃加氢的潜力。通过分析八种金属(单价、双价、三价和四价)和七种配体的组合,我们描述了金属-配体相互作用对氢化活性的影响。我们的研究结果强调,催化活性主要取决于金属离子的电荷和大小。虽然二价 Ae 金属阳离子分别微妙地调节反应物和产物的结合和释放,为该反应提供适当的平衡,但配体在决定其催化活性方面只起次要作用。我们展示了如何利用火山图快速筛选预期的 Ae 催化剂,以建立指导方针以实现促进氢化过程的最大活性。配体在决定其催化活性方面只起次要作用。我们展示了如何利用火山图快速筛选预期的 Ae 催化剂,以建立指导方针以实现促进氢化过程的最大活性。配体在决定其催化活性方面只起次要作用。我们展示了如何利用火山图快速筛选预期的 Ae 催化剂,以建立指导方针以实现促进氢化过程的最大活性。

更新日期:2021-08-26
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