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

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将硝酸水溶液转化为有用或良性产品（如氨）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。拟议的研究通过开发强大而高效的电催化剂来解决这个问题，通过还原化学将硝酸盐转化为所需的化合物。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换的其他电催化剂的开发。外展活动包括与公共广播节目“A Moment of Science”的合作以及制作有关氮循环的 YouTube 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，致力于开发与环境相关的电催化剂。石墨共轭大环配合物的模块化类别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 射线光谱法。与经过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，计算方法可以提供对不同氧化态电子结构的详细了解。除了用于机械询问的标准电化学和计算方法之外，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。对硝酸盐还原选择性材料的机理研究将提供见解，有望有助于合理设计具有改进活性的催化剂。外展活动包括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，让公众广泛了解电催化及其在开发环境有益的还原氮化学方面的实用性。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力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, 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.