Collaborative Proposal: NSF-DFG Echem: Understanding the Mechanism of Urea Oxidation on Nickel-Based Electrocatalysts

合作提案：NSF-DFG Echem：了解镍基电催化剂上尿素氧化的机制

• 批准号: 2054933
• 负责人: Liney Arnadottir
• 金额: $ 36.23万
• 依托单位: Oregon 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: 2021-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2054933&HistoricalAwards=false
• 关键词: Collaborative; Proposal; NSF; DFG; Echem

Urea – a common high-nitrogen chemical waste product of mammalian metabolism, and a major component of fertilizer – poses significant threat to water resources from agricultural run-off and municipal wastewater. A promising means for removing excess urea is to oxidize it electrochemically to produce produce harmless compounds. Urea removal processes can also be used to generate electricity and to produce hydrogen for fuel cells. Electrochemical urea removal therefore exhibits strong potential as a transformative technology by converting a harmful waste product to the benefit of society, industry, and the environment. The project brings together researchers from the United States and Germany to apply a synergistic blend of experimental and theoretical methods to the study of electrochemical urea removal from water. In particular, the project seeks fundamental understanding of catalytic urea oxidation that is needed to develop feasible urea removal technologies. Effective urea removal systems are key to a large number of technological applications including municipal and agricultural wastewater treatment, remediation of fertilizer run-off, ammonia synthesis, hydrogen production, and electricity generation. Other benefits from this project will include workforce development and educational outreach to underrepresented grade-school students. These efforts will promote increased diversity in STEM fields, a student exchange program between Germany and the US, and improved scientific literacy of the general public.The goal of this research project is to develop comprehensive knowledge of electrochemical urea removal over nickel-based catalysts, based on experimental and theoretical research spanning molecular and device levels. Electrochemical urea removal will be studied by density functional theory calculations, vibrationally and electronically resonant sum frequency spectroscopy, and electrochemical measurements of reaction rate and product distributions. Particular attention will be paid to the active form of the nickel oxide electrode as it exists in different phases and oxidation states depending on electrode potential and history, such as aging and preparation method. This combined electrochemical, spectroscopic, and computational approach provides insight related to catalyst structural changes and how they affect the urea reaction mechanism, reactivity, and effectiveness of nickel, nickel-iron, and nickel-chromium catalysts. The outcomes of this research will greatly advance the scientific understanding of electrochemical urea removal -- about which little is known -- and establish a foundation in the wider field of electrocatalysis regarding electrochemical reactions on oxide surfaces and on surfaces that undergo a change in oxidation state as part of the overall reaction mechanism. Successful completion of this research will benefit society through sustainable methods for treating wastewater and agricultural run-off that will reduce demand on water supply systems and enhance the biodiversity of marine ecosystems. This project was awarded through the “NSF-DFG Lead Agency Activity in Electrosynthesis and Electrocatalysis (NSF-DFG EChem)" opportunity, a collaborative solicitation that involves the National Science Foundation and Deutsche Forschungsgemeinschaft (DFG).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.

尿素 - 哺乳动物代谢的常见高氮化学废物，也是肥料的主要组成部分 - 对农业径流和市政废水的水资源具有重大威胁。去除过量尿素的一种有希望的方法是用电化学上的氧化物产生无害的化合物。尿素去除过程也可用于发电并为燃料电池生产氢。因此，电化学尿素去除通过将有害废物转换为社会，工业和环境的利益，从而表现出强大的变革技术潜力。该项目汇集了来自美国和德国的研究人员，将实验和理论方法的协同融合到从水中去除电化学尿素的研究中。特别是，该项目寻求对开发可行尿素去除技术所需的催化尿素氧化的基本理解。有效的尿素去除系统是大量技术应用的关键，包括文化和农业废水处理，肥料径流的修复，氨合成，氢生产和发电。该项目的其他好处将包括为不足的成绩学生提供劳动力发展和教育宣传。这些努力将促进STEM领域的多样性，这是德国与美国之间的学生交流计划，并改善了公众的科学文献。该研究项目的目的是基于基于实验性和理论研究跨度分子和设备水平的基于镍的催化剂的电化学尿素去除对基于镍的催化剂的全面知识。电化学尿素去除将通过密度功能理论计算，虚拟和电子谐振总和频率光谱以及反应速率和产品分布的电化学测量结果进行研究。特别注意镍氧化物电极的活性形式，因为它以不同的相位和氧化状态存在，具体取决于电极电位和历史，例如衰老和制备方法。这种结合的电化学，光谱和计算方法提供了与催化剂结构变化有关的见解，以及它们如何影响镍，镍铁和镍铬催化剂的尿素反应机理，反应性和有效性。这项研究的结果将大大提高对电化学尿素去除的科学理解 - 几乎没有知名度 - 并在氧化物表面和在氧化物表面上的电化学反应的广泛领域建立基础，这些反应是整体反应机制的一部分。成功完成这项研究将通过可持续的方法来治疗废水和农业径流，从而使社会受益，这将减少对供水系统的需求并增强海洋生态系统的生物多样性。该项目是通过“ NSF-DFG电力合成和电催化领域的主要活动（NSF-DFG Echem）”机会授予的，这是一种协作征求，涉及国家科学基金会和Deutsche forschungsche forschungsgemeinschaft（DFG）。影响审查标准。