Functionalization of Inorganic Materials as Heterogeneous Catalyst for Selective Oxidation Reactions

在这个研究项目中，我们创造了一种有效的方法来设计非均相纳米结构催化剂，使用层状粘土材料（羟基磷灰石、蒙脱土和水滑石）作为大配体，以分子氧作为氧化剂进行选择性氧化，碳-碳键形成反应和一锅合成。我们发现，我们的催化系统，包括非均相金属催化剂，可以在实现简单和清洁的材料转化方面提供显著的好处，因为它们具有以下优点：(i)它们允许使用无污染的氧化剂，（ii）它们具有高催化活性和选择性，（iii）它们允许简单的后处理程序和催化剂的容易回收，(v)它们是可回收的，（iv）它们允许一锅顺序反应。通过应用配位化学的概念，我们开发了一种纳米结构金属的制备方法，比以前的固体负载金属催化剂的合成方法简单得多，并为制备催化活性位点提供了强有力的方案。

In this research project, we created an effective approach to designing heterogeneous nano-structured catalysts using layered-clay materials (hydroxyapatite, montmorillonite, and hydrotalcite) as macroligands for selective oxidations using molecular oxygen as an oxidant, carbon-carbon bond-forming reactions, and one-pot syntheses.We found that our catalytic systems including the heterogeneous metal catalysts can offer significant benefits in achieving simple and clean materials transformation because they have the following advantages: (i) they allow the use of non-polluting oxidants, (ii) they possess high catalytic activity and selectivity, (iii) they allow a simple work-up procedure and easy recovery of the catalyst, (v) they are recyclable, and (iv) they allows one-pot sequential reaction. By applying concepts from coordination chemistry, we have developed a preparation for nano-structured metal species that is much simpler than previous synthetic methods for solid-supported metal catalysts, and provides a strong protocol for preparing catalytically active sites.