NSF-DFG Echem: Operando Electronic Structure Determination of Iron and its Time-Dependent Dynamics in FexNi100-x(OH)y Electrooxidation Catalysts

NSF-DFG Echem：FexNi100-x(OH)y 电氧化催化剂中铁的操作电子结构测定及其随时间变化的动力学

• 批准号: 2055245
• 负责人: Lauren Greenlee
• 金额: $ 38万
• 依托单位: University of Arkansas
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-07-15 至 2021-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2055245&HistoricalAwards=false
• 关键词: NSF; DFG; Echem; Operando; Electronic

This project aims to identify the structure of iron within iron-nickel hydroxide catalyst materials. These materials are highly active electrocatalysts for key reactions important to next-generation energy conversion and storage, including water electrolysis to produce hydrogen and battery electrodes. Understanding the chemistry of the iron species underpins the overall goal of designing and synthesizing non-precious metal electrocatalysts to support our future energy economy. These electrocatalyst materials will also likely play a role in other future electrochemical technologies, including chemical conversion and upcycling, biomass conversion, water treatment, and resource recovery. As such, this project, and its pursuit of understanding how iron structure changes in the electrochemical environment, is critical to support national energy security, as well as to advance society toward clean energy technologies. Discoveries made will support a wide range of research activities focused on similar non-precious metal oxides and hydroxides, advancing not only the science of iron-nickel hydroxides but of other similar materials and of synchrotron-based spectroscopy techniques aimed at probing catalyst materials in their operating environments. This U.S.-German collaboration will also strengthen international scientific relationships and contribute to the development of a diverse, globally competitive science and engineering workforce.The overarching research goal of this proposal is to experimentally probe Fe electronic structure under alkaline electrooxidation conditions by combining materials expertise with the x-ray spectroscopy instrumentation and expertise. Collaboratively conducted operando experiments will allow the team to unequivocally describe electronic state(s) of Fe and to understand the time dependency and hysteresis of Fe structural changes in FexNi100-x(OH)y nanocatalysts. The electrocatalytic reaction of focus will be the alkaline oxygen evolution reaction (OER). This project will further scientific understanding of the chemical and electronic structure of the active site for the OER in these catalysts, as well as advance fundamental understanding of Fe in the operando electrooxidative environment. The project will study a series of FexNi100-x(OH)y films and subsequently nanoparticle FexNi100-x(OH)y catalysts with soft x-ray absorption spectroscopy, x-ray emission spectroscopy, and resonant inelastic x-ray scattering. The project will focus on the iron L-edge and the oxygen K-edge of selected materials, and will include development of an operando cell for spectroscopy experiments, as well as detailed electrochemical analysis and in vacuo characterization of the catalyst materials.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.

该项目旨在确定铁 - 尼克尔氢氧化物催化剂材料中铁的结构。这些材料是对下一代能量转换和存储重要的关键反应的高度活性电催化剂，包括水电解以产生氢和电池电极。了解铁物种的化学基础是设计和综合非贵金属电催化剂以支持我们未来的能源经济的总体目标。这些电催化剂材料也可能在其他未来的电化学技术中发挥作用，包括化学转化和升级，生物量转化，水处理和资源回收。因此，该项目及其追求了解铁结构在电化学环境中的变化对于支持国家能源安全以及向清洁能源技术推动社会至关重要。发现的发现将支持广泛的研究活动，这些研究活动集中在类似的非偏心金属氧化物和氢氧化物上，不仅可以推进铁 - 尼克尔氢氧化物的科学，而且还提高了其他类似材料和基于同步加速器的光谱技术的科学，旨在探测其操作环境中催化剂材料的科学。这项美国 - 德国合作还将加强国际科学关系，并为多样性，全球竞争性的科学和工程劳动力的发展做出贡献。该提案的总体研究目标是通过将含X射线光谱仪器和专业知识结合材料的材料将材料专业知识结合起来，在酗酒的电氧化条件下实验探测FE电子结构。协作进行的操作实验将使团队明确描述FE的电子状态，并了解FexNi100-X（OH）Y纳米催化剂中Fe结构变化的时间依赖性和滞后。焦点的电催化反应将是碱性氧气进化反应（OER）。该项目将进一步科学地理解这些催化剂中OER活性位点的化学和电子结构，以及对操作汇总电氧化环境中FE的基本了解。该项目将研究一系列具有软X射线抽象光谱，X射线发射光谱和谐振X射线X射线散射的FEXNI100-X（OH）Y膜和随后的纳米颗粒FEXNI100-X（OH）Y催化剂。 The project will focus on the iron L-edge and the oxygen K-edge of selected materials, and will include development of an operando cell for spectroscopy experiments, as well as detailed electrochemical analysis and in vacuum characterization of the catalyst materials.This project was awarded through the “NSF-DFG Lead Agency Activity in Electrosynthesis and Electrocatalysis (NSF-DFG EChem)” opportunity, a Collaborative Solicitation这涉及国家科学基金会和德意志Forschungsgemeinschaft（DFG）。该奖项反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的影响审查标准，被视为通过评估来获得珍贵的支持。