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.

尿素是哺乳动物代谢过程中常见的高氮化学废物，也是肥料的主要成分，它对农业径流和城市废水中的水资源构成了重大威胁，一种去除过量尿素的有前景的方法是通过电化学氧化来生产尿素。产生无害的化合物。尿素去除工艺还可用于发电和生产用于燃料电池的氢气，通过将有害的废物转化为有益的物质，具有作为变革性技术的巨大潜力。该项目汇集了来自美国和德国的研究人员，将实验和理论方法相结合，研究电化学去除水中的尿素。开发可行的尿素去除技术所需的有效尿素去除系统是许多技术应用的关键，包括城市和农业废水处理、化肥径流修复、氨合成、氢气生产和该项目的其他好处包括劳动力发展和对代表性不足的小学生的教育推广，这些努力将促进 STEM 领域的多样性、德国和美国之间的学生交流计划以及提高公众的科学素养。该研究项目的目标是基于跨越分子和器件水平的实验和理论研究，通过密度泛函理论计算、振动和电子共振来研究电化学尿素去除的综合知识。特别关注氧化镍电极的活性形式，因为它根据电极电势和历史（例如老化和制备方法）而存在不同的相和氧化态。这种结合电化学、光谱和计算的方法提供了与催化剂结构变化以及它们如何影响镍、镍铁和镍铬的尿素反应机制、反应性和有效性相关的见解。这项研究的成果将极大地推进对电化学尿素去除的科学理解（对此知之甚少），并为氧化物表面和发生变化的表面上的电化学反应的更广泛的电催化领域奠定基础。氧化态作为整体反应机制的一部分。这项研究的成功完成将通过可持续的方法处理废水和农业径流，从而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，从而造福社会。 “NSF-DFG电合成和电催化牵头机构活动 (NSF-DFG EChem)”机会，这是一项涉及美国国家科学基金会和德国研究协会 (DFG) 的合作招标。该奖项反映了 NSF 的法定使命，并通过使用基金会的评估进行评估，被认为值得支持。智力价值和更广泛的影响审查标准。