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

f 元素和 d(0) 催化剂介导的原子效率杂原子转化

• 批准号: 2247666
• 负责人: Tobin Marks
• 金额: $ 60万
• 依托单位: Northwestern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2247666&HistoricalAwards=false
• 关键词: Atom; Efficient; Heteroatom; Transformations; Mediated

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.

在化学系化学催化计划的支持下，西北大学的Tobin Marks教授正在发现，理解和优化用于三种不同类型的关键有机反应的f元素和d（0）-过渡金属催化剂。据估计，催化剂支撑着美国国内生产总值的约35%，大规模生产涂料，肥料，燃料，塑料，药品，医疗服装和设备以及其他化学品。在未来，催化转化必须更加节能和资源高效，无毒，无污染，并在更具选择性，可持续性和经济竞争力的技术中使用低成本，地球上丰富的金属。Marks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青年科学家解决全球规模的问题，同时在广泛的学科领域进行前沿研究。该奖项资助的项目涉及催化剂创造，催化剂评估和理解催化产品形成的途径的跨学科，教育严格的组合。这些活动与高度互动的研究小组环境相结合，为研究生，本科生和博士后学者提供了出色的培训/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。假设驱动的主题利用地球丰富的镧系元素，锕系元素和早期过渡金属络合物的独特性质。首先，正在研究一种使用简单的镧系元素催化剂和易于处理的硼化合物的碳元素多重键的非常快速和选择性的还原过程，用于新的合成应用，以促进获得天然产品，药物和精细化学品。在第二个主题中，催化性稀土金属在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，大的镧系元素导致吡啶双键结构的变化，而小的镧系元素导致吡啶外围的取代。在第三个主题中，正在研究锆烯烃聚合催化剂对具有胺、膦和硫醚官能团的单体的共聚的耐受性，并探索所得材料的性质。这项研究的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的内置表面抗菌，抗病毒和抗真菌特性提供新的途径。该奖项反映了NSF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。