Collaborative Research: CAS: Graphite-Conjugated Macrocycle Electrocatalysts for Nitrate Reduction

合作研究：CAS：石墨共轭大环电催化剂用于硝酸盐还原

• 批准号: 2102497
• 负责人: Elena Jakubikova
• 金额: $ 29.38万
• 依托单位: North Carolina State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-06-01 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102497&HistoricalAwards=false
• 关键词: Collaborative; Research; CAS; Graphite; Conjugated

With the support of the Chemical Catalysis program in the Division of Chemistry, Professor Yulia Pushkar of Purdue University, Professor Jeremy Smith of Indiana University and Associate Professor Elena Jakubikova of North Carolina State University are studying catalysts that will use electrical energy for the conversion of aqueous nitrate to useful or benign products such as ammonia. Nitrate is a water pollutant that occurs largely as a result of agricultural fertilizer use. The proposed research takes a first step to addressing this problem through the development of robust and efficient electrocatalysts that to convert nitrate to desirable compounds via reductive chemistry. Scientific insights gained through these studies will likely impact the development of other electrocatalysts for other useful electrochemical conversions. Outreach activities include a partnership with the public radio program “A Moment of Science” and the development of YouTube videos on the nitrogen cycle.This project combines the expertise of three research groups in synthetic, electrochemical, spectroscopic, and computational studies on the development of environmentally relevant electrocatalysts. A modular class of graphite-conjugated macrocyclic complexes will be characterized by a range of physical methods, including synchrotron-based X-ray spectroscopy. Together with experimentally calibrated electronic structure calculations, these data will provide information on the coordination environment, structure, and electron configuration of the metal ion. Redox properties will be characterized by electrochemical measurements, with computational methods providing detailed insights into the electronic structures of different oxidation states. In addition to standard electrochemical and computational methods for mechanistic interrogation, in situ spectroscopic characterization is expected to provide detailed information on the nature of intermediates in the catalytic cycle. Mechanistic investigations into materials that are selective for nitrate reduction will provide insight that is expected to aid in the rational design of catalysts having improved activity. Outreach activities are to including a partnership with a public radio broadcast and the development of publicly accessible educational videos are expected to reach a wide audience and inform the public broadly about electrocatalysis and its utility in developing environmentally beneficial reductive nitrogen chemistry.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.

在化学系化学催化项目的支持下，普渡大学的 Yulia Pushkar 教授、印第安纳大学的 Jeremy Smith 教授和北卡罗来纳州立大学的 Elena Jakubikova 副教授正在研究利用电能转化水相的催化剂。硝酸盐是一种水污染物，主要是由于农业肥料的使用而产生的，该研究迈出了通过开发稳健的方法来解决这一问题的第一步。通过这些研究获得的科学见解可能会影响其他有用的电化学转化的电催化剂的开发，包括与公共广播节目“A Moment of Science”的合作。该项目结合了三个研究小组在合成、电化学、光谱和计算研究方面的专业知识，开发环境相关的电催化剂。石墨共轭大环配合物将通过一系列物理方法进行表征，包括基于同步加速器的X射线光谱学以及经过实验校准的电子结构计算，这些数据将提供有关金属的配位环境、结构和电子构型的信息。氧化还原性质将通过电化学测量来表征，除了用于机械询问的标准电化学和计算方法之外，计算方法还可以提供对不同氧化态电子结构的详细了解。表征有望提供有关催化循环中中间体性质的详细信息，对硝酸盐还原选择性的材料的机理研究将提供有助于合理设计具有改进活性的催化剂的见解。与公共广播电台合作以及开发可公开访问的教育视频预计将覆盖更广泛的受众，并让公众广泛了解电催化及其在开发对环境有益的还原氮化学方面的效用。该奖项反映了 NSF 的法定使命，并被视为值得通过使用基金会的智力优点和更广泛的影响审查标准进行评估来支持。