Organometallic Chemistry, Catalysis and Molecular Materials

本申请的主要焦点在于开发用于通过使用环境友好的“绿色”氧化剂，特别是氧气和过氧化氢来选择性氧化烃的催化剂。 该领域的最大挑战是开发用于甲烷选择性氧化为甲醇的催化剂。 甲烷是一种可以通过管道运输的气体，对发电或供暖非常有用，但不容易用于为移动的车辆提供动力。 甲醇是一种更适合于此目的的液体，它也是合成其他化学品的更有价值的原料，因此在该企业中取得成功的动机很大。 其他烷烃和芳烃的选择性绿色氧化在减少污染的同时也将对经济有很大的好处。 当然，这是一个难题，有一个激烈的，全球性的研究努力来解决它。我们的方法是研究铂和钯化合物的潜在催化作用的各个步骤。 最重要的步骤是烷烃或芳烃的碳-氢键活化，氧化剂的氧-氧键活化和氧化烃的还原消除。 挑战在于了解是什么影响了每个反应步骤的难易程度，并找到一种促进所有这些步骤的催化剂。 我们将利用我们在有机金属化学的合成，反应性和机理方面的专业知识，推动这一领域的发展。第二个重点是进一步发展用于合成大环、低聚或聚合分子材料的动态开环聚合领域。 我们计划利用我们在这一领域的专业知识，使钯，铂和金的低聚化合物的合成应用于氧化催化项目，但它也适用于传感和光子材料等不同领域，因此开发合成原理对材料科学具有长期利益。

The main focus of this application is on development of catalysts for the selective oxidation of hydrocarbons by using environmentally friendly “green” oxidants, notably oxygen and hydrogen peroxide. The greatest challenge in this field is to develop a catalyst for selective oxidation of methane to methanol. Methane is a gas which can be transported by pipeline and is very useful for power generation or heating, but it is not easily used to power mobile vehicles. Methanol is a liquid which is much better suited to this purpose, and it is also a more valuable feedstock for synthesis of other chemicals, so there is a great incentive to succeed in this enterprise. Selective green oxidation of other alkanes and arenes would also be of great benefit to the economy, while reducing pollution. Naturally, this is a difficult problem and there is an intense, global research effort to solve it. Our approach is to study individual steps in the potential catalysis by platinum and palladium compounds. The most important steps are carbon-hydrogen bond activation of the alkane or arene, oxygen-oxygen bond activation of the oxidant, and reductive elimination of the oxidized hydrocarbon. The challenge is to understand what affects the ease of each reaction step, and to find a catalyst which facilitates all of them. We will use our expertise in synthesis, reactivity and mechanism in organometallic chemistry to push this field forward.******The secondary focus is to further develop the area of dynamic ring-opening polymerization for the synthesis of macrocyclic, oligomeric or polymeric molecular materials. We plan to use our expertise in this field to enable synthesis of oligomeric compounds of palladium, platinum and gold to apply in the oxidation catalysis project, but it is also applicable in diverse areas such as sensing and photonic materials, so developing the synthetic principles has long term benefits in materials science.*****