Collaborative Research: Controlling Metal-Oxide Interface Chemistry for New C-H Activation Catalysts

合作研究：控制新型 C-H 活化催化剂的金属-氧化物界面化学

• 批准号: 2329470
• 负责人: Bert Chandler
• 金额: $ 34万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-12-15 至 2026-11-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2329470&HistoricalAwards=false
• 关键词: Collaborative; Research; Controlling; Metal; Oxide

The world will continue to rely on hydrocarbon resources during the Clean Energy Transition to renewable and sustainable net-zero carbon fuels and chemicals. Thus, there is a substantial opportunity to reduce the carbon footprint of our Nation’s tremendous natural gas reserves through efficient chemical processing to manufacture readily transportable liquid fuels and chemicals. The project addresses a key challenge in natural gas chemical processing – breaking the carbon-hydrogen bonds as needed to manufacture higher-value fuels and chemicals. Catalytic technology is critical to energy efficient natural gas upgrading. To that end, the project investigates a new class of hydrocarbon conversion catalysts that can potentially enable natural gas to be converted to liquid fuels and chemicals in the field, thereby generating enormous boosts in energy efficiency and a significant reduction in greenhouse gas emissions. The project also will invest in research experiences targeted to economically disadvantaged undergraduate students, who are disproportionately women and under-represented minorities. The undergraduates will be engaged in a peer-mentoring network, which can be particularly effective in promoting undergraduate success, especially when the students in the team have diverse cultural and socio-economic backgrounds. The project will combine the investigators’ experimental and computational expertise to develop new heterolytic C-H activation catalysts based on the unique properties of Au/oxide interfaces, which will be tuned to maximize activity by varying the composition of the oxide. A combination of density functional theory and new in-situ IR techniques will be employed to quantify H2 activation parameters over a carefully chosen series of Au/MOx catalysts. H-H and C-H bond activation are closely related processes, so the broad approach is to first study how oxide composition tunes the thermodynamics and kinetics of H2 activation, and then extend this knowledge to design effective interfaces for C-H activation. Machine learning techniques will use these results to survey H2 activation chemistry for thousands of oxide compositions, which will provide direct insight into underlying physio-chemical processes that govern complex interactions at the metal-oxide interface. Coupled with experiments intentionally designed to inform and refine the computational models, the research will go beyond identification of factors that impact C-H activation (such as support reducibility, support basicity, M-OH bond flexibility) to assess the relative impact of each system variable. The resulting C-H bond activation chemistry will be tested with a suite of hydrocarbons chosen for their adsorption properties and with catalytic benzyl alcohol oxidation. Ideally, the project will generate a research protocol that will combine efficient computational screening and experimental validation of metal-support catalyst combinations tailored for efficient C-H bond activation across a broad range of hydrocarbon and organic molecules.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.

在清洁能源向可再生和可持续的净零碳燃料和化学品转型期间，世界将继续依赖碳氢化合物资源，因此，有很大的机会通过高效的化学加工来减少我国巨大天然气储量的碳足迹。该项目解决了天然气化学加工中的一个关键挑战——根据需要打破碳氢键以制造更高价值的燃料和化学品，这对于节能天然气升级至关重要。结束，项目研究一种新型碳氢化合物转化催化剂，该催化剂有可能使天然气在现场转化为液体燃料和化学品，从而大幅提高能源效率并显着减少温室气体排放。该项目还将投资于研究经验。针对经济上处于不利地位的本科生，其中女性和少数族裔比例过高。本科生将参与同伴指导网络，这对于促进本科生的成功特别有效，特别是当团队中的学生具有不同的文化和背景时。社会经济该项目将结合研究人员的实验和计算专业知识，开发基于金/氧化物界面独特性质的新型异解C-H活化催化剂，通过改变氧化物的组成和密度组合来调整催化剂以最大限度地提高活性。功能理论和新的原位红外技术将用于量化一系列精心选择的 Au/MOx 催化剂上的 H2 活化参数，H-H 和 C-H 键活化是密切相关的过程，因此广泛的方法是首先研究氧化物的组成。调整 H2 活化的热力学和动力学，然后扩展这些知识来设计有效的 C-H 活化界面。机器学习技术将使用这些结果来调查数千种氧化物成分的 H2 活化化学，这将提供对基础物理化学的直接了解。结合控制金属-氧化物界面上复杂相互作用的实验，该研究将超越影响 C-H 活化的因素（例如载体还原性、载体碱度、M-OH）的范围。键灵活性）来评估每个系统变量的相对影响，将使用一系列根据吸附特性选择的碳氢化合物和催化苯甲醇氧化来测试所得的 C-H 键活化化学。将计算有效筛选和实验验证相结合，对金属载体催化剂组合进行定制，以实现广泛碳氢化合物和有机分子中 C-H 键的有效活化。该奖项是 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准。