Organometallic Chemistry of Heterocycles

杂环有机金属化学

• 批准号: 1360985
• 负责人: William Jones
• 金额: $ 42万
• 依托单位: University of Rochester
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1360985&HistoricalAwards=false
• 关键词: Organometallic; Chemistry; Heterocycles

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor William Jones of the University of Rochester is examining new reactions that can be used to make organic compounds of interest in biology and the pharmaceutical industry. To accomplish this, fundamental reactions of transition metal catalysts are being examined that can be used to form heterocycles from readily available, inexpensive starting materials. Professor Jones is also examining new catalysts that can break open heterocycles and allow their structures to be altered.The broader impacts of this work include outreach to high school students to attract interest to careers in STEM related fields, as well as the development of new processes for routes to intermediates of pharmaceutical importance. The combination of a detailed physical-organometallic background combined with an understanding of how to apply modern computational methods to these problems produces extremely well trained scientists for the US chemical industry. One specific goal of this project is to examine fundamental aspects of cyclometallation via the "Concerted Metallation-Deprotonation" pathway that is now popular in organic synthetic methodology to produce heterocycles. These cyclometallation studies are revealing fundamental aspects of how these molecules effect the chemical transformations, and are providing insight into the control of the selectivity that is critical to formation of the desired product. A second goal is to develop uses for the now commonly observed transition metal based carbon-sulfur bond cleavage sulfur-containing molecules. One application involves anchoring a reversible carbon-sulfur activation catalyst to a solid support that allows this material to act as a "sulfur sponge," thereby permitting the cleanup of hydrocarbon fuels prior to combustion.

在这个由化学部化学催化项目资助的项目中，罗切斯特大学的威廉·琼斯教授正在研究可用于制造生物学和制药工业感兴趣的有机化合物的新反应。为了实现这一目标，正在研究过渡金属催化剂的基本反应，这些反应可用于从容易获得、廉价的起始材料形成杂环。 琼斯教授还在研究可以打破杂环并改变其结构的新催化剂。这项工作的更广泛影响包括向高中生推广，以吸引他们对 STEM 相关领域的职业兴趣，以及开发具有药物重要性的中间体路线的新工艺。 详细的物理有机金属背景与对如何应用现代计算方法解决这些问题的理解相结合，为美国化学工业培养了训练有素的科学家。该项目的一个具体目标是通过“协同金属化-去质子化”途径来研究环金属化的基本方面，该途径目前在生产杂环的有机合成方法中很流行。 这些环金属化研究揭示了这些分子如何影响化学转化的基本方面，并提供了对选择性控制的深入了解，这对于所需产物的形成至关重要。 第二个目标是开发现在常见的基于过渡金属的碳硫键断裂含硫分子的用途。 一种应用涉及将可逆碳硫活化催化剂锚定到固体载体上，使该材料充当“硫海绵”，从而允许在燃烧之前净化碳氢化合物燃料。

项目成果

Synthesis, characterization, and reactivity of Cp*Rh(III) complexes having functional N,O chelate ligands

• DOI: 10.1016/j.jorganchem.2017.02.015
• 发表时间: 2017-10
• 期刊: Journal of Organometallic Chemistry
• 影响因子: 2.3
• 作者: Lloyd Munjanja;Hong-Zhong Yuan;W. Brennessel;W. Jones