Transition metal chemistry and catalysis

加氢催化剂被工业用于生产燃料、散装化学品和精细化学品，包括药品、农用化学品和香料。它们通常由昂贵、稀有和有毒的铂金属组成。自2007年以来，我们的团队已经发现并发明了可持续和更便宜的铁催化剂，有望取代一些用于酮和亚胺不对称氢化生产有价值的醇和胺的传统催化剂。例如，某些醇可用于合成用于化疗的药物，某些胺可用于合成抗抑郁药和抗生素。廉价的铁催化剂也可能在能源领域的二氧化碳加氢以及氢的储存和释放中找到应用。建议进一步发现有用的催化剂结构并充分了解它们，以便对绿色化学工业至关重要的替代过程能够成功。提出了多种新的、高效的合成方法，可用于高通量筛选催化剂。催化剂将在温和的条件下由新的和已知的模块形成，其中铁离子作为模板。一个感兴趣的成分是n -杂环碳（NHC）供体，因为它允许催化剂合成而不使用有毒的磷化氢试剂。我们已经发现了用于酯加氢的活性NHC催化剂，这可能会使硼和铝还原剂的浪费使用过时。确定催化剂是均相还是非均相是很重要的。我们在2012年报道了第一个使用铁纳米颗粒进行不对称催化的例子，该纳米颗粒是由铁前驱体的均相溶液形成的。我们将使用最先进的实践和理论方法来探索我们的新催化剂系统的功能。这项工作还可能导致发现利用阳光将水分解成氢燃料和氧的催化剂，以及有效合成聚酰胺的催化剂。

Hydrogenation catalysts are used by industry to produce fuels, bulk chemicals and fine chemicals including pharmaceuticals, agrochemicals and fragrances. They are usually composed of expensive, rare and toxic platinum metals. Since 2007 our group has discovered and invented sustainable and much cheaper iron catalysts that promise to replace some conventional catalysts used for the asymmetric hydrogenation of ketones and imines for the production of valuable alcohols and amines. For example, certain alcohols can be used for the synthesis of drugs used in chemotherapy, and selected amines, in the synthesis of antidepressants and antibiotics. Cheap iron catalysts might also find application in the energy field in the hydrogenation of carbon dioxide as well as hydrogen storage and evolution. It is proposed to discover further useful catalyst structures and fully understand them so that this replacement process, vital for a greener chemical industry, can be successful. A variety of new, efficient syntheses are proposed that are amenable to high throughput screening of catalysts. Catalysts will be formed from novel and known modules under mild conditions where the iron ion acts as a template. A component of interest is the N-heterocyclic carbene (NHC) donor since this allows catalyst synthesis without the use of toxic phosphine reagents. We have discovered active NHC catalysts for ester hydrogenation that might make obsolete the wasteful use of boron and aluminum reductants. It is important to determine whether the catalysts are homogeneous or heterogeneous. We reported in 2012 the first example of asymmetric catalysis using iron nanoparticles that are formed from a homogeneous solution of iron precursor. We will use state of the art practical and theoretical methods to probe the functioning of our new catalyst systems. This work might also lead to the discovery of catalysts that use sunlight to split water into hydrogen fuel and oxygen and catalysts for the efficient synthesis of polyamides.