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.

在清洁能源过渡到可再生和可持续的零碳燃料和化学物质期间​​，世界将继续依靠碳氢化合物资源。通过有效的化学加工来制造易于传播的液态燃料和化学物质，可以减少美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主要挑战 - 生产高价值燃料和化学物质的需要打破碳氢键。催化技术对于节能天然气升级至关重要。为此，该项目研究了一类新的碳氢化合物转化催化剂，该催化剂可能有可能使天然气转化为田间的液态燃料和化学物质，从而在能源效率方面产生巨大的提升，并显着降低温室气体排放。该项目还将投资于针对经济不利的本科生的研究经验，这些学生是女性不成比例的，代表性不足的少数群体。本科生将参与同行网络，这在促进本科生的成功方面特别有效，尤其是当团队中的学生具有不同的文化和社会经济背景时。该项目将结合研究人员的实验和计算专业知识，以基于AU/氧化物界面的独特特性开发新的杂化C-H活化催化剂，这将通过改变氧化物的组成来调整以最大化活性。密度功能理论和新的原位IR技术的结合将用于量化精心选择的AU/MOX催化剂系列的H2激活参数。 H-H和C-H键激活是密切相关的过程，因此广泛的方法是首先研究氧化物组成如何调整H2激活的热力学和动力学，然后将此知识扩展到设计有效的C-H激活接口。机器学习技术将使用这些结果来调查成千上万种氧化物组成的H2激活化学，这将直接洞悉基本的生理化学过程，该过程控制金属氧化物界面上复杂的相互作用。再加上有意旨在告知和完善计算模型的实验，这项研究将超越影响C-H激活的因素（例如支持降低，支持碱性，M-OH键灵活性），以评估每个系统变量的相对影响。所得的C-H键激活化学将通过选择的碳氢化合物和催化苄醇氧化来测试。 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 precious of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.