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

在化学系化学催化项目的支持下，耶鲁大学的王海亮和宾厄姆顿大学的朱利安·帕内蒂尔正在研究使用可再生电力将二氧化碳和硝酸盐转化为甲胺的化学反应，这两种物质都是主要的环境污染物，甲胺是一种在化学合成，制药，农业和航空航天工业中具有广泛应用的有机化合物。这种转化有望在温和的条件下将环境废物回收为有价值的化学产品。在该项目中，团队将联合收割机实验和计算研究相结合，系统研究电催化反应的机理。在基本机理理解的指导下，该团队将致力于开发更具选择性和活性的催化剂，并优化最佳催化剂，以提高实际应用的反应性能。该项目还将提供化学教育机会，重点是催化和可持续性，通过外联活动，课堂教学和研究培训，为STEM的各种学生提供教育机会。（科学、技术、工程和数学）领域。根据该奖项，耶鲁大学的王海亮和宾厄姆顿大学的朱利安·帕内蒂尔正在研究电化学合作，碳纳米管负载酞菁钴分子催化水介质中二氧化碳和硝酸盐还原为甲胺。本计画的目标是了解催化剂的反应机制，并改善反应效能。该团队将结合联合收割机理论计算、动力学研究和原位振动光谱测量来分析反应机理。将确定选择性和限速步骤及其影响因素。将检查关键反应中间体和C-N偶联步骤。在增强机制理解的指导下，分子结构剪裁，纳米级相互作用和微环境调整将结合起来，为最有效和可持续的合成工艺开发最佳催化系统。该项目还将通过外展活动、课堂教学和研究培训为STEM领域的多样化学生提供化学教育机会，重点是催化和可持续性。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。

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.