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

在化学系化学催化计划的支持下，普渡大学的Yulia Pushkar教授，印第安纳州大学的Jeremy Smith教授和北卡罗来纳州州立大学的Elena Jakubikova副教授正在研究将电能用于将硝酸盐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。拟议的研究迈出了解决这一问题的第一步，通过开发强大而有效的电催化剂，通过还原化学将硝酸盐转化为所需的化合物。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其他电催化剂的开发。外联活动包括与公共广播节目"科学时刻"建立伙伴关系，以及制作关于氮循环的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，以开发与环境相关的电催化剂。一个模块类的石墨共轭大环配合物将其特征在于一系列的物理方法，包括同步加速器为基础的X射线光谱。与实验校准的电子结构计算一起，这些数据将提供关于金属离子的配位环境、结构和电子构型的信息。氧化还原特性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了解。除了标准的电化学和计算方法的机械询问，在原位光谱表征，预计将提供详细的信息，在催化循环中的中间体的性质。对硝酸盐还原选择性材料的机理研究将提供预期有助于具有改进活性的催化剂的合理设计的见解。推广活动包括与公共广播电台的合作，以及开发公众可访问的教育视频，这些活动预计将接触到广泛的受众，并向公众广泛宣传电催化及其在开发对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，并被认为值得通过利用基金会的知识价值和更广泛的评估来支持。影响审查标准。

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.