Multiconfigurational methods for copper cluster catalysts in copper-exchanged zeolites involved in methane-to-methanol conversion

美国拥有大量的天然气储量，而这种天然气的主要成分是甲烷。将甲烷运输到可以用来制造燃料和化学品的地方是昂贵的。将甲烷转化为甲醇，一种易于运输的液体，是解决这个问题的一种方法。为了在经济上可行，甲烷转化为甲醇必须是高效的。它还必须在使用氧气（空气）和实际条件下发生。为了使该反应具有经济效益，需要改进催化剂。科学家们还没有发现如何改进这些催化剂，这仍然是一个未解决的问题和一个活跃的研究领域。在这个项目中，内华达大学里诺分校的Samuel Odoh博士正在开发和使用计算化学方法来准确地了解这些催化剂的工作原理以及如何改进它们。为解决这一问题而开发的新的计算方法也可以应用于化学和催化中的其他问题。正在开发的技术和软件将提供给研究界。Odoh博士和他的团队正在为来自内华达州北部弱势群体和低收入家庭的学生提供教育和研究机会。这些活动包括让高中生在Odoh博士的实验室进行暑期研究实习，以及向里诺-太浩的市中心地区进行拓展和招聘活动。这些活动正在改善初中、高中和大学的科学、技术、工程和数学教育。在化学部门化学催化项目的资助下，内华达大学里诺分校的Odoh博士正在对铜交换沸石的性质如何决定它们的活性、周转率和在温和温度条件下甲烷与氧氧化形成甲醇的选择性进行基本的了解。基于理论的对这些催化平台的物理和化学性质的理解可以导致对具有更好的甲烷-甲醇转化（MMC）性能的材料的改进预测。研究人员正在开发和使用新的和现有的量子力学方法，能够准确地描述金属氧化物簇的多参考特性，这些簇是MMC的活性位点。这些方法被用来研究铜交换沸石中活性位点的性质和特征。Odoh博士的实验室正在对这些材料中的MMC和副反应提供更深入的了解。本研究为设计更好的催化剂提供了指导，并为MMC催化剂的发展指明了方向。此外，正在开发的计算技术和软件将提供给研究界，用于解决化学和催化方面的其他问题。Odoh博士积极参与STEM外展项目，专注于招募来自低收入家庭和代表性不足背景的学生。这是通过高中生研究实习、指导驱动和教育工作者发展来实现的，以支持项目的更广泛影响。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。

The United States has large reserves of natural gas, and the major component of this natural gas is methane. Methane is expensive to transport to locations where it can be utilized to make fuels and chemicals. Conversion of methane to methanol, a liquid and easily transported material, is one solution to this problem. To be economically feasible, the conversion of methane to methanol must be efficient. It must also occur using oxygen (air) and under practical conditions. Improved catalysts are needed for this reaction to be economically useful. Scientists have not yet discovered how to improve these catalysts, and it remains an unsolved problem and an active area of research. In this project, Dr. Samuel Odoh of the University of Nevada Reno is developing and using computational chemistry methods to understand exactly how these catalysts work and how to improve them. The new computational approaches being developed to solve this problem also have applications to other problems in chemistry and catalysis. The techniques and software being developed will be provided to the research community. Dr. Odoh and his group are providing education and research opportunities students from underrepresented groups and low-income families in Northern Nevada. These activities include summer research internships for high school students in Dr. Odoh's laboratory as well as outreach and recruitment drives to the inner-city areas of Reno-Tahoe. These activities are improving science, technology, engineering, and mathematics education at the middle school, high school and college levels.With funding from the Chemical Catalysis Program of the Chemistry Division, Dr. Odoh of the University of Nevada Reno, is developing fundamental understanding of how the properties of copper-exchanged zeolites dictate their activity, turnover rates and selectivity in the oxidation of methane with oxygen to form methanol under mild temperature conditions. A theory-based understanding of the physical and chemical properties of these catalytic platforms can lead to improved predictions of materials with better performance for methane-to-methanol conversion (MMC). The researchers are developing and using new and existing quantum-mechanical methods capable of accurately describing the multireference properties of the metal oxide clusters that are the active sites for MMC. These methods are being used to investigate the nature and identity of the active sites in copper-exchanged zeolites. Dr. Odoh's laboratory is providing greater understanding of MMC and side-reactions in these materials. This work is guiding the design of better catalysts and leading to a pivot in the direction of developing catalysts for MMC. In addition, the computational techniques and software being developed will be provided to the research community for use in attacking other problems in chemistry and catalysis. Dr. Odoh is actively engaged in STEM outreach programs focused on recruiting students from low-income families and under-represented backgrounds. This is being done through high school student research internships, mentoring drives and educator development in support of the broader impacts of the project.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.