LEAPS-MPS: Taming the Radicals-Manipulating Lattice-Confined Metalloradicals for C-H Activation

LEAPS-MPS：驯服自由基操纵晶格限制的金属自由基以实现 C-H 激活

• 批准号: 2213401
• 负责人: Wenyang Gao
• 金额: $ 25万
• 依托单位: New Mexico Institute of Mining and Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-09-01 至 2023-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2213401&HistoricalAwards=false
• 关键词: LEAPS; MPS; Taming; Radicals; Manipulating

This award is funded in whole or in part under the American Rescue Plan Act of 2021 (Public Law 117-2). In this project, funded by the Mathematical and Physical Sciences Directorate and housed in the Chemistry Division, Professor Wenyang Gao and his students at New Mexico Institute of Mining and Technology will take advantage of the high reactivities of chemicals known as radicals (i.e. molecules that have odd numbers of electrons) and apply them to promote reactions of light hydrocarbons. Advances in hydraulic fracturing technologies provide vast available reserves of domestic light hydrocarbons, e.g., natural gas. Insufficient processing infrastructure coupled with the challenge of long-range transportation of gaseous hydrocarbons has prevented efficient utilization of these resources. A significant amount of natural gas has to be burned in on-site flares to avoid its direct atmospheric release. Chemical upgrading of light hydrocarbons, for instance, transforming gaseous methane into liquid methanol, is expected to turn these resources into chemical fuels or industrial feedstocks that have increased ease of handling, transport, and storage. Prof. Gao’s work will address the lack of chemical approaches for transforming methane efficiently and selectively by trapping highly reactive metal-containing radicals in rigid porous materials known as metal-organic frameworks, which will facilitate the desired reactions of light hydrocarbons. Meanwhile, the project will engage underrepresented minority students working on addressing sustainability and energy-related issues and prepare them as role models for the future scientific workforce.The project will take advantage of the high reactivities of radicals and apply them for the activation of light hydrocarbons. Prof. Gao and his students will utilize metal-organic frameworks, and their lattice confinement effect, to tame the highly reactive metalloradicals and utilize these species for hydrocarbon conversion. This project expects to provide synthetic access to solid-state radicals, examine their structures and reactivities, and obtain understanding on how tamed radicals to impact the chemical valorization of light hydrocarbons. This project will not only develop novel synthetic chemistry to access lattice-confined metalloradicals in the solid state, but also examine these highly reactive metalloradicals towards activating strong C(sp3)–H bonds in simple hydrocarbons.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.

该奖项全部或部分根据2021年美国救援计划法案（公法117-2）资助。 在这个由数学和物理科学理事会资助并设在化学系的项目中，新墨西哥州矿业与技术学院的高文阳教授和他的学生将利用被称为自由基（即具有奇数电子的分子）的化学物质的高反应性，并将其应用于促进轻质烃的反应。水力压裂技术的进步提供了国内轻质烃的巨大可用储量，例如，天然气.处理基础设施不足，加上气态烃远距离运输的挑战，阻碍了这些资源的有效利用。大量的天然气必须在现场燃烧，以避免其直接释放到大气中。轻质烃的化学升级，例如将气态甲烷转化为液态甲醇，预计将这些资源转化为化学燃料或工业原料，从而增加了处理、运输和储存的便利性。高教授的工作将解决缺乏有效和选择性地转化甲烷的化学方法的问题，方法是在称为金属有机框架的刚性多孔材料中捕获高活性含金属的自由基，这将促进轻质烃的所需反应。 与此同时，该项目将吸引少数民族学生参与解决可持续性和能源相关问题，并将他们培养为未来科学工作者的榜样。该项目将利用自由基的高反应性，并将其应用于轻烃的活化。高教授和他的学生将利用金属有机框架及其晶格限制效应来驯服高活性金属自由基，并利用这些物种进行烃转化。该项目预计将提供固态自由基的合成途径，检查其结构和反应性，并了解驯服的自由基如何影响轻质烃的化学稳定。 该项目不仅将开发新型合成化学，以获得固态晶格限制的金属自由基，还将研究这些高活性金属自由基对激活简单烃中的强C（sp3）-H键的作用。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。