NSF-BSF: Towards a Molecular Understanding of Dynamic Active Sites in Advanced Alkaline Water Oxidation Catalysts

NSF-BSF：高级碱性水氧化催化剂动态活性位点的分子理解

• 批准号: 2400195
• 负责人: Shannon Boettcher
• 金额: $ 60万
• 依托单位: University of Oregon Eugene
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-06-01 至 2027-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2400195&HistoricalAwards=false
• 关键词: NSF; BSF; Towards; Molecular; Understanding

With the support of the Chemical Catalysis program in the Division of Chemistry, Professor Shannon Boettcher of University of Oregon, Eugene is studying the chemistry of catalytic materials for high-efficiency, low-cost generation of green hydrogen from electrically driven water splitting. This research is motivated in part by a grand challenge in the field known as the hydrogen shot, with the target of reaching the production of hydrogen fuel at $1 per 1 kg within one decade. Green hydrogen is obtained as the product of one-half of the overall water splitting reaction. The other half, water oxidation, limits the overall efficiency of hydrogen generation and must be accelerated by earth-abundant catalysts to improve rates and lower costs. Boettcher’s group has developed several catalysts based on nickel, iron, and cobalt with efficient water oxidation ability that are promising for hydrogen technologies. With this grant, his group will study with molecular precision the underlying chemical principles and structures that dictate the high performance of these catalysts and whether these chemical principles hold under industry-relevant conditions. This will be done by leveraging academic partnerships that facilitate rapid access to advanced surface characterization and computational techniques, and practical feedback from industrial collaborators. In addition to supporting work which will have a high impact on the field of catalysis, this grant will also provide key training to graduate and undergraduate students soon to enter the burgeoning renewable energy workforce, facilitate the continuation of educational outreach among students from the middle school to undergraduate level.Under this award, Professor Shannon Boettcher and his research team are studying fundamental chemical descriptors for advanced alkaline water-oxidation catalysts. Water oxidation is characterized by slow kinetics and represents a key constraint in the performance of large-scale hydrogen production through water electrolysis. This oxidation reaction typically occurs on the surface of heterogeneous oxides/oxyhydroxides that are poorly defined, which makes relating structural, compositional, and electronic features to observed activity difficult. Fundamental catalysis science discoveries can address these challenging relations and, importantly, translate learned principles into improved technology for alkaline hydrogen production. With this grant, Prof. Boettcher and his team are building a fundamental understanding of active-site generation, retention, and loss for record-activity earth-abundant Fe-Ni/Co oxyhydroxides. Specifically, they will (1) study how the structure and properties of newly proposed surface Fe-oxo cluster active sites drive high activity in these transition-metal oxyhydroxides; (2) develop chemical descriptors to explain surface restructuring and activation of crystalline oxides (vs. amorphous oxides) for the oxygen evolution reaction (OER); and (3) understand if and how dynamic catalyst surfaces and Fe-based active sites drive record OER catalysis in high-temperature concentrated electrolyte conditions. The work seeks to build a more complete, temperature-dependent, thermodynamic and kinetic understanding of the materials and surface processes central to water oxidation at industrially relevant conditions. These aims will be studied through a combination of computation and experiment, with a significant focus on experiments conducted under operating conditions. Collaborative computational efforts by Prof. Maytal Caspary-Toroker at the Technion in Haifa, Israel, funded separately by the U.S.-Israel Binational Science Foundation, is expected to provide new and more accurate approaches to modeling the thermodynamics and kinetic processes in these complex oxyhydroxides.This collaborative US/Israel project is supported by the US National Science Foundation and the Israel Binational Science Foundation.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.

在化学催化计划中，俄勒冈大学的Shannon Boettcher教授在化学催化计划的支持下，Eugene正在研究催化材料的化学，以进行高效，低成本的绿色氢从电驱动的水分解中。这项研究的一部分是由称为氢射击的领域的巨大挑战所激发的，其目标是在1千克的情况下以每1公斤的价格达到氢燃料的生产。获得绿色氢作为总体水分拆分反应的一半的产物。另一半是水氧化，限制了氢产生的总体效率，必须通过土壤丰富的催化剂加速以提高速率和降低成本。 Boettcher的小组已经开发了几种基于镍，铁和钴的催化剂，具有有效的水氧化能力，这些催化剂可以用于氢技术。有了这项赠款，他的小组将以分子精度学习，基本的化学原理和结构决定了这些催化剂的高性能以及这些化学原理是否在与行业相关的条件下成立。这将通过利用学术合作伙伴关系来完成，从而有助于快速获得高级表面特征和计算技术，以及工业合作者的实际反馈。除了支持将对催化领域产生重大影响的工作外，这项赠款还将为研究生和本科生提供重要的培训，以便很快进入新兴的可再生能源劳动力，从而促进了从中学的学生继续进行教育外展活动，从该奖项授予该奖项。水氧化的特征是缓慢的动力学，代表了通过水电解生产大规模氢的关键限制。这种氧化反应通常发生在定义较差的异质氧化物/氧化氧化物的表面上，这使得与观察到的活性变得困难。基本的催化科学发现可以解决这些挑战关系，并重要的是，将学习的原理转化为改进的酒精氢生产技术。有了这项赠款，Boettcher教授和他的团队正在建立对活跃的地球活性Earth Earth Earth Earth Fe-Ni/Co羟基氧化物的基本理解。具体而言，他们将（1）研究新提出的表面Fe-oxo簇活性位点的结构和性能如何在这些过渡金属氧化物中驱动高活性； （2）开发化学描述符，以解释氧气进化反应（OER）的晶体氧化物（与无定形氧化物）的表面修发和激活； （3）了解动态催化剂表面和基于Fe的活性位点是否以及如何在高温浓缩电解质条件下驱动OER催化。这项工作旨在建立对材料和表面过程的更完整，依赖温度，热力学和动力学理解，这是在工业相关条件下水氧化的中心。这些目标将是通过计算和实验的结合进行研讨会，重点是在操作条件下进行的实验。预计由美国 - 以色列双国科学基金会分别资助的以色列海法技术的Maytal Caspary-Torker教授的合作计算努力有望提供新的，更准确的方法，以建模这些复杂的氧化氧化物中的热力学和动力学过程。反映了NSF的法定任务，并通过使用基金会的知识分子和更广泛的影响审查标准评估来诚实地表示支持。