NSF-DFG Echem: CAS: Hydrofunctionalization of Alkenes by non-Redox Paired Electrocatalysis

在化学系化学催化项目的支持下，康奈尔大学的宋琳正在与德国奥尔登堡的卡尔·冯·奥西茨基大学的合作者沿着研究非氧化还原成对电催化烯烃的对映选择性加氢官能化。Lin研究小组的目标是开发用于合成增值有机化合物的电催化过程。该研究计划的长期目标是促进可推广的电催化过程的发展或在合成化学中的广泛影响，并可能应用于新型药物，农用化学品和催化剂的立体控制合成。这些重要的化合物中有许多含有碳-卤素键和碳-碳键。本研究的目标是建立高效，选择性和可持续的反应技术，以促进使用丰富的原料化学品形成碳-卤素和碳-碳键。电化学是一种直接利用电力驱动化学反应的过程，本质上是一种高效、选择性和可持续的技术。催化的引入可以进一步提高电化学反应的能量效率，并提供控制最终产物的产率和特性的机会。该项目位于有机合成，催化和电化学的界面。因此，它也非常适合各级科学家的教育。除了促进科学知识的进步和改善精细化工生产外，该项目还将通过与德国团队的研究和国际合作对学生的培训产生更广泛的影响。该项目通过“NSF-DFG电合成和电催化牵头机构活动（NSF-DFG EChem）”机会获得资助，这是一个涉及NSF和德国研究共同体（DFG）的合作征集活动。康奈尔大学的宋琳与德国奥尔登堡的卡尔·冯·奥西茨基大学的合作者一起，正在开发烯烃加氢官能化的电催化方法。拟议的研究将争取配对电解与氧化还原活性金属催化的组合，使双催化中间体的产生，以实现所需的氢官能化反应。两个目标将同时进行，包括（一）建立非氧化还原成对的电催化氢氯化的背景下，和（二）非氧化还原成对的电催化使用电分析和光谱工具的机理研究。在获得初步的原理证明后，新的催化策略将进一步扩展到氢氯化以外的其他类型的氢官能化反应。最后，林博士团队将开发一个电化学短期课程，旨在教育缺乏电化学经验的有机化学家，并为他们提供建立自己的电解实验所需的知识和指导。这个奖项反映了NSF的法定使命，并通过使用基金会的智力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, Song Lin of Cornell University is studying the enantioselective hydrofunctionalization of alkenes by non-redox paired electrocatalysis along with collaborators at Carl von Ossietzky University Oldenburg in Germany. The Lin research group aims to develop electrocatalytic processes for the synthesis of value-added organic compounds. The long-term objective of this research program is to facilitate the development of a generalizable electrocatalytic process or wide impact in synthetic chemistry, with possible application in the stereocontrolled synthesis of building blocks for new pharmaceuticals, agrochemicals, and catalysts. Many of these important compounds contain carbon-halogen and carbon-carbon bonds. The goal of this research is to establish efficient, selective, and sustainable reaction technologies that will promote the formation of carbon-halogen and carbon-carbon bonds using abundant feedstock chemicals. Electrochemistry—a process that directly uses electricity to drive chemical reactions—is an intrinsically efficient, selective, and sustainable technology. The introduction of catalysis can further augment the energy efficiency of electrochemical reactions and offer opportunities to control the yield and identity of the end product. The project lies at the interface of organic synthesis, catalysis, and electrochemistry. Therefore, it is also well suited for the education of scientists at all levels. In addition to contributing to the advancement of scientific knowledge and improving fine chemical manufacturing, the project will also exert broader impacts on the training of students through research and international collaboration with the German team. The project is being funded through the "NSF-DFG Lead Agency Activity in Electrosynthesis and Electrocatalysis (NSF-DFG EChem)" opportunity, a collaborative solicitation that involves NSF and Deutsche Forschungsgemeinschaft (DFG).Together with collaborators at Carl von Ossietzky University Oldenburg in Germany, Song Lin of Cornell University is developing electrocatalytic methods for the hydrofunctionalization of alkenes. The proposed research will enlist the combination of paired electrolysis with redox-active metal catalysis to enable the generation of dual catalytic intermediates to achieve the desired hydrofunctionalization reactions. Two objectives will be pursued simultaneously, including (i) establishing non-redox paired electrocatalysis in the context of hydrochlorination and (ii) mechanistic investigation of non-redox paired electrocatalysis using electroanalytical and spectroscopic tools. Upon obtaining initial proof of principle, the new catalytic strategy will be further expanded to other types of hydrofunctionalization reactions beyond hydrochlorination. Finally, the Lin team will develop an electrochemical short course that aims to educate organic chemists with little electrochemistry experience and provide them with the knowledge and guidance needed to set up their own electrolysis experiments.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.