CAS: Nitrogen-Coupled Carbon Dioxide Conversion to Methylamine: Molecular Level Understanding and Tailoring of the Electrocatalysis

CAS：氮耦合二氧化碳转化为甲胺：分子水平上电催化的理解和定制

• 批准号: 2154724
• 负责人: Hailiang Wang
• 金额: $ 54.74万
• 依托单位: Yale University
• 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: 2022-08-01 至 2025-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154724&HistoricalAwards=false
• 关键词: CAS; Nitrogen; Coupled; Carbon; Dioxide

With the support of the Chemical Catalysis program in the Division of Chemistry, Hailiang Wang of Yale University and Julien Panetier of Binghamton University are studying chemical reactions that use renewable electricity to transform carbon dioxide and nitrate, both of which are major environmental pollutants, into methylamine, an organic compound that has widespread applications in chemical synthesis, pharmaceuticals, agriculture, and the aerospace industry. This transformation holds promise for recycling environmental wastes into valuable chemical products under mild conditions. In this project, the team will combine experimental and computational research to systematically study the mechanism of the electrocatalytic reaction. With the guidance of fundamental mechanistic understanding, the team will work to develop more selective and active catalysts, as well as optimize the best catalysts to improve reaction performance toward practical applications. This project will also provide educational opportunities in chemistry, with a focus on catalysis and sustainability, via outreach activities, classroom teaching, and research training to a diverse body of students in STEM (science, technology, engineering and mathematics) fields.Under this award, Hailiang Wang of Yale University and Julien Panetier of Binghamton University are studying the electrochemical co-reduction of carbon dioxide and nitrate in aqueous media to methylamine catalyzed by cobalt phthalocyanine molecules supported on carbon nanotubes. The goal of this project is to understand the catalytic mechanism and improve the reaction performance. The team will combine theoretical calculations, kinetic studies, and in situ vibrational spectroscopy measurements to analyze the reaction mechanism. Selectivity- and rate-limiting steps, as well as their contributing factors, will be identified. Key reaction intermediates and the C-N coupling step will be examined. With guidance from enhanced mechanistic understanding, molecular structure tailoring, nanoscale interactions, and microenvironment tuning will be combined to develop the best catalytic systems for the most efficient and sustainable synthetic processes achievable. This project will also provide educational opportunities in chemistry, with a focus on catalysis and sustainability, via outreach activities, classroom teaching, and research training to a diverse body of students in STEM fields.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.

在化学催化计划的支持下，耶鲁大学的Hailiang Wang和宾厄姆顿大学的Julien Panetier正在研究使用可再生电力转化二氧化碳和硝酸盐的化学反应，这两种反应都是主要环境污染物，具有甲基胺的主要环境，是化学物质的，是化学典型的，是一种化学典型的属性，是一种化学典型的综合属性，是一种化学典型的应用。航空业。这种转变有望在轻度条件下将环境废物回收为有价值的化学产品。在该项目中，团队将结合实验和计算研究，以系统地研究电催化反应的机制。在基本机械理解的指导下，团队将致力于开发更多的选择性和活跃的催化剂，并优化最佳的催化剂，以提高针对实际应用的反应性能。该项目还将通过外展活动，课堂教学和研究培训来提供化学方面的教育机会，重点关注催化和可持续性，并向STEM（科学，技术，工程和数学）领域的多元化学生进行研究。由碳纳米管支撑的钴邻苯二甲胺分子催化的甲胺。该项目的目的是了解催化机制并改善反应性能。该团队将结合理论计算，动力学研究和原位振动光谱测量，以分析反应机制。将确定选择性和限制性步骤及其贡献因素。将检查关键反应中间体和C-N耦合步骤。通过增强机械理解的指导，将结合使用分子结构调整，纳米级相互作用和微环境调整，以开发最佳和可持续的合成过程最佳的催化系统。该项目还将通过外展活动，课堂教学和研究培训来提供化学方面的教育机会，重点关注催化和可持续性，并向STEM领域的各种学生进行研究培训。这项奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛的影响来通过评估来支持的。