RII Track-4:NSF: In-Situ/Operando Characterizations of Single Atom Catalysts for Clean Fuel Generation

该项目将与美国阿贡国家实验室（ANL）合作，研究用于电化学过程的带电表面上的单原子催化剂（SACs）的结构、行为和动态变化。这些原子分散的催化剂高效、稳定、价格低廉，在清洁燃料发电技术方面具有巨大的潜力。该项目将利用ANL先进光子源（APS）提供的尖端x射线吸收精细结构吸收设施。通过将这种强大的原位/operando x射线吸收光谱（XAS）与高灵敏度、快速响应的电化学质谱（EC-MS）相结合，研究团队将探测绿色制氢和二氧化碳转化电化学过程中SACs的动态行为和变化，以及电解质中催化剂附近的局部微环境。从这项研究中获得的知识有可能推动减缓气候危机和清洁能源生产的科学和技术。该项目将提供跨多个领域的多学科教育，如光谱学、材料工程、表面科学和电化学。此外，它为研究生、本科生和高中生提供了一个宝贵的机会，为能源和环境领域的进步做出积极贡献。这个研究基础设施改进轨道4 EPSCoR研究研究员（RII轨道4）项目将为肯塔基大学研究基金会的一名副教授提供奖学金，并为一名研究生提供培训。这项工作将与阿贡国家实验室的研究人员合作进行。该研究小组将与美国科学院的科学家合作。他们将共同开发先进的原位/operando光谱技术，以揭示以前无法获得的信息，包括：(1)对催化剂结构、团聚/重构和活化/失活的见解；(2)实时观测局部电解质环境的动态变化；(3)复杂反应途径的探索。由于对贵金属或非贵金属原子的有效利用，SACs可以显著降低电化学器件的制造和维护成本。SACs具有明确的单原子活性位点排列，是研究催化剂行为和局部环境的理想平台。对SACs结构、行为和命运的研究将通过以下具体任务来组织，旨在揭示这些过程的基本方面：学习x射线吸收光谱技术并进行非原位XAS来检查单原子催化剂的结构和局部环境；建立电化学制氢过程的原位x射线吸收光谱；并在电化学过程中同时结合operando x射线光谱和EC-MS进行析氢和二氧化碳转化。该项目将重点研究两种特定的sac，即单独分散在过渡金属二硫化物载体上的铂原子和碳网络中与氮配位的铜原子。研究小组的目标是获得关于绿色氢气生产和二氧化碳转化过程中单个或簇状催化剂原子的结构、分布、行为和变化的革命性知识。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

In partnership with Argonne National Laboratory (ANL), this project will investigate the structure, behavior, and dynamic change of single atom catalysts (SACs) on electrified surface for use in electrochemical processes. These atomically dispersed catalysts are efficient, stable, and affordable and they hold immense potential for clean fuel generation technologies. The project will harness the cutting-edge X-ray absorption fine structure absorption facilities available at ANL’s Advanced Photon Source (APS). By combining this powerful in-situ/operando X-ray absorption spectroscopy (XAS) with highly sensitive, fast-responding electrochemical mass spectrometry (EC-MS), the research team will probe the dynamic behavior and change of SACs as well as local microenvironments adjacent to catalysts in electrolyte during electrochemical processes of green hydrogen production and carbon dioxide conversion. The knowledge gained from this research has potential to advance the science and technology for climate crisis mitigation and clean energy production. The project will offer a multidisciplinary education that spans diverse fields, such as spectroscopy, materials engineering, surface science and electrochemistry. Moreover, it presents a valuable opportunity for graduate, undergraduate, and high-school students to actively contribute to advancements in the energy and environmental sectors. This Research Infrastructure Improvement Track-4 EPSCoR Research Fellows (RII Track-4) project will provide a fellowship to an Associate professor and training for a graduate student at the University of Kentucky Research Foundation. This work will be conducted in collaboration with researchers at Argonne National Laboratory. The research team will collaborate scientists at the APS. Together, they will develop advanced in-situ/operando spectroscopic techniques to unveil previously inaccessible information, including (1) insights into catalyst structure, agglomeration/reconstruction, and activation/deactivation; (2) real-time observations of dynamic changes in local electrolyte environment; and (3) exploration of complicated reaction pathways. Owing to the efficient utilization of noble or non-noble metal atoms, SACs can dramatically reduce manufacturing and maintenance costs of electrochemical devices. SACs have the well-defined arrangement of active sites involving single atoms, serving as an ideal platform for studying catalyst behaviors and local environments. The investigation of SACs structure, behavior and fate will be organized through the following specific tasks, designed to uncover the fundamental aspects of these processes: learning X-ray absorption spectroscopic technique and conducting ex-situ XAS to examine the structure and local environment of single-atom catalysts; establishing in-situ X-ray absorption spectroscopy during electrochemical hydrogen production; and combining operando X-ray spectroscopy with EC-MS simultaneously during electrochemical processes for hydrogen evolution and carbon dioxide conversion. This project will focus on two specific SACs, namely platinum atoms individually dispersed on transition metal dichalcogenide support and copper atoms coordinated with nitrogen in a carbon network. The research team aims to gain transformative knowledge about the structure, distribution, behavior, and changes of single or clustered catalyst atoms during green hydrogen production and carbon dioxide conversion.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.