Homogeneous/heterogeneous approach to catalysis using nanoparticles

我们研究计划的主要目标是设计新的催化剂，以便在对环境影响最小的情况下进行有效的合成。催化现在几乎普遍应用于化学和石化过程中。催化也很快在绿色化学中占据了中心位置，因为它的优点：更低的能源消耗，更少的原料用量，更少的有毒物质的使用，更高的预期产品收率，以及减少有害溶剂的使用。我们将通过在纳米粒子科学和配位化学之间的接口工作来寻求这些目标，以提供新的催化系统。通过这种方法，我们利用金属配体在配位化学中的广泛应用，来修饰、增强和探测金属纳米粒子的催化活性。首先，我们将研究金属纳米粒子的结构/活性关系，重点是保护金属核心的配体的电子性质和周围环境的影响。我们将合成一个金属纳米库(Au，Rh，Pd，...)与各种不同的配体，如硫醇、亚膦、亚磷酸或胺。这个文库将被用来评估催化过程的结构/反应相关性。氢甲酰化和炔烃活化将是我们的主要目标之一。我们还将研究离子液体作为纳米粒子催化溶剂的潜力，目的是提高反应活性并允许串联反应。其次，我们将使用有前景的催化剂来实现重要的转移加氢反应，特别是在C=C和三键上。

The main goal of our research programme is to design new catalysts for efficient synthesis with minimal environmental impact. Catalysis is now almost universally used in chemical and petrochemical processes. Catalysis has also quickly assumed a central place in Green Chemistry because of its benefits: lower energy consumption, lesser quantities of starting materials, lesser use of toxic materials, higher yield of the desired product, and decreased use of deleterious solvents. We will seek those goals by working at the interface between nanoparticle science and coordination chemistry to provide new catalytic systems. With this approach, we take advantage of the versatile and well-explored properties of metal ligands as they are used in coordination chemistry to modify, enhance and probe catalytic activity of metal nanoparticles. Firstly, we will investigate the structure/activity relationships in metal nanoparticles, emphasising the impact of the electronic properties of the ligands protecting the metallic core and of the surrounding environment. We will synthezise a library of metal nanoparticles (Au, Rh, Pd, ...) with a variety of different ligands such as thiols, phosphines, phosphites or amines. This library will be use to assess the structure/reactivity dependence of catalytic processes. Hydroformylation and alkyne activation will be among our major goals. We will also investigate the potential of ionic liquids as a solvent for catalysis with nanoparticles, with the aim to enhance reactivity and allow tandem reactions. Secondly, we will use promising catalysts to effect important transfer hydrogenation reactions, especially on C=C and triple bonds.