Atom-Efficient Heteroatom Transformations Mediated by f-Element and d(0) Catalysts

在化学系化学催化项目的支持下，西北大学的Tobin Marks教授正在为三种不同类型的关键有机反应发现、理解和优化f元素和d(0)过渡金属催化剂。据估计，催化支撑了大约35%的美国GDP，大规模生产涂料、化肥、燃料、塑料、药品、医疗服装和设备以及其他化学品。在未来，催化转化必须更具能源和资源效率，无毒，无污染，并在更具选择性，可持续和经济竞争力的技术中使用低成本，地球丰富的金属。马克斯教授和他的研究小组正在通过开发f元素和d(0)催化剂来解决这些重要的挑战，这些催化剂推进了构建和修饰有机分子的新方法。这些活动还有助于教育年轻科学家在进行跨广泛学科领域的前沿研究的同时，解决全球规模的问题。该奖项资助的项目涉及跨学科、教育上严格的催化剂创造、催化剂评估和对催化产物形成途径的理解。这些活动结合了高度互动的研究小组环境，为研究生、本科生和博士后学者提供了优秀的培训/指导，这些学者将从事工业、国家实验室或学术事业，特别强调妇女和代表性不足的少数民族的参与。该奖项支持的研究项目围绕三个高度整合的探索性、假设驱动的主题，利用地球上丰富的镧系元素、锕系元素和早期过渡金属配合物的独特特性。首先，使用简单的镧系催化剂和易于处理的硼化合物，正在研究一种非常快速和选择性的碳元素多键还原过程，以促进天然产品，药品和精细化学品的新合成应用。在第二个主题中，催化稀土金属在元素周期表中的位置被用来引导反应结果。当应用于对药物和精细化学品很重要的吡啶分子时，大的镧系元素会导致吡啶双键结构的变化，而小的镧系元素会导致吡啶外围的取代。在第三个主题中，研究了锆烯烃聚合催化剂对单体与胺、膦和硫醚官能团共聚的耐受性，并探讨了所得材料的性能。这项研究更广泛的长期科学影响包括为一次性ppe甚至医院服装和口罩提供内置表面抗菌、抗病毒和抗真菌特性的新途径。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Tobin Marks of Northwestern University is discovering, understanding, and optimizing, f-element and d(0)-transition metal catalysts for three different types of critical organic reactions. It is estimated that catalysis underpins approximately 35% of the U.S. GDP, producing coatings, fertilizers, fuels, plastics, pharmaceuticals, medical garments and equipment, and other chemicals on a vast scale. In the future, catalytic transformations must be more energy and resource efficient, non-toxic, non-polluting, and employ low-cost, earth-abundant metals in more selective, sustainable, and economically competitive technologies. Professor Marks and his research group are addressing these important challenges with the development of f-element and d(0) catalysts that advance new ways to build and modify organic molecules. These activities are also serving to educate young scientists to attack global-scale problems, while conducting forefront research across broad disciplinary fields. Projects funded by this award involve a transdisciplinary, educationally rigorous combination of catalyst creation, catalyst evaluation, and understanding the pathways by which catalytic products are formed. These activities combined with a highly interactive research group environment, provide excellent training/mentoring for graduate, undergraduate, and postdoctoral scholars bound for industrial, national laboratory, or academic careers, with special emphasis on participation by women and underrepresented minorities.The research program supported by this award is configured around three highly-integrated exploratory, hypothesis-driven themes capitalizing on the unique properties of earth-abundant lanthanide, actinide, and early transition metal complexes. In the first, a remarkably rapid and selective reduction process for carbon-element multiple bonds using simple lanthanide catalysts and easy to handle boron compounds is being investigated for new synthetic applications to facilitate access to natural products, pharmaceuticals and fine chemicals. In the second theme, the position of catalytic rare earth metals in the periodic table is being used to steer reaction outcomes. When applied to pyridine molecules, which are important for drugs and fine chemicals, large lanthanides lead to a change in the pyridine double bond structure whereas small lanthanides lead to substitution on the pyridine periphery. In the third theme, the tolerance of zirconium olefin polymerization catalysts towards the copolymerization of monomers with amine, phosphine and thioether functional groups is being investigated and the properties of the resulting materials explored. The broader long term scientific impact of this research includes the potential provide new routes to build-in surface anti-bacterial, anti-viral, and anti-fungal characteristics for disposable PPEs and even hospital clothing and face masks.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.