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教授和北卡罗莱纳州立大学的Elena Jakubikova副教授正在研究一种催化剂，这种催化剂将利用电能将硝酸水转化为有用的或良性的产物，如氨。硝酸盐是一种主要由于农业肥料的使用而产生的水污染物。提出的研究通过开发强大而高效的电催化剂，通过还原化学将硝酸盐转化为所需的化合物，迈出了解决这个问题的第一步。通过这些研究获得的科学见解可能会影响用于其他有用电化学转化的其他电催化剂的开发。外联活动包括与公共广播节目“科学一刻”建立伙伴关系，以及在YouTube上制作关于氮循环的视频。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，以开发与环境相关的电催化剂。模块化的一类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。与实验校准的电子结构计算一起，这些数据将提供有关金属离子的配位环境，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，计算方法提供了对不同氧化态电子结构的详细见解。除了用于机械分析的标准电化学和计算方法外，原位光谱表征有望提供有关催化循环中中间体性质的详细信息。对硝酸还原选择性材料的机理研究，将有助于合理设计具有更高活性的催化剂。外联活动将包括与公共无线电广播建立伙伴关系，并制作可公开观看的教育录象带，预期将使广大听众了解电催化及其在发展对环境有益的还原氮化学方面的用途。该奖项反映了美国国家科学基金会的法定使命，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。