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

铜交换沸石中铜簇催化剂参与甲烷转化为甲醇的多构型方法

基本信息

批准号：
1800387
负责人：
Samuel Odoh
金额：
$ 40万
依托单位：
Board of Regents, NSHE, obo University of Nevada, Reno
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-07-01 至 2023-06-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800387&HistoricalAwards=false
关键词：
Multiconfigurational methods copper cluster catalysts

项目摘要

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.

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。将甲烷运输到可用于制造燃料和化学品的地点是昂贵的。将甲烷转化为甲醇（一种液体且易于运输的材料）是该问题的一种解决方案。为了在经济上可行，甲烷向甲醇的转化必须高效。它也必须使用氧气（空气）和在实际条件下进行。为了使该反应在经济上有用，需要改进的催化剂。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，内华达州里诺大学的Samuel Odoh博士正在开发和使用计算化学方法来准确了解这些催化剂的工作原理以及如何改进它们。为解决这个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。奥多博士和他的小组正在为来自北方内华达州代表性不足的群体和低收入家庭的学生提供教育和研究机会。这些活动包括在奥多博士的实验室为高中生提供暑期研究实习机会，以及在里诺-太浩市中心地区开展外联和招聘活动。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。在化学系化学催化计划的资助下，内华达州里诺大学的奥多博士正在对铜交换沸石的性质如何决定其活性进行基本的了解，在温和的温度条件下用氧气氧化甲烷形成甲醇的转换率和选择性。对这些催化平台的物理和化学性质的基于理论的理解可以改进对具有更好甲烷至甲醇转化（MMC）性能的材料的预测。研究人员正在开发和使用新的和现有的量子力学方法，能够准确描述金属氧化物簇的多参考特性，这些金属氧化物簇是MMC的活性位点。这些方法被用来研究铜交换沸石中活性中心的性质和身份。Odoh博士的实验室正在提供对MMC和这些材料中的副反应的更多了解。这项工作是指导更好的催化剂的设计，并导致在MMC的催化剂开发方向的一个支点。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领域的其他问题。Odoh博士积极参与STEM外展计划，重点是从低收入家庭和代表性不足的背景中招募学生。这是通过高中学生的研究实习，指导驱动器和教育工作者的发展，以支持该项目的更广泛的影响。这个奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

项目成果

期刊论文数量（13）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Methane C–H Activation by [Cu 2 O] 2+ and [Cu 3 O 3 ] 2+ in Copper-Exchanged Zeolites: Computational Analysis of Redox Chemistry and X-ray Absorption Spectroscopy

铜交换沸石中 [Cu 2 O] 2 和 [Cu 3 O 3 ] 2 的甲烷 C–H 活化：氧化还原化学和 X 射线吸收光谱的计算分析

DOI：
10.1021/acs.inorgchem.0c03693
发表时间：
2021
期刊：
Inorganic Chemistry
影响因子：
4.6
作者：
Suleiman, Olabisi;Panthi, Dipak;Adeyiga, Olajumoke;Odoh, Samuel O.
通讯作者：
Odoh, Samuel O.

Building on the strengths of a double-hybrid density functional for excitation energies and inverted singlet-triplet energy gaps

建立在激发能双杂化密度泛函和反单线态-三线态能隙的优势之上

DOI：
10.1063/5.0133727
发表时间：
2023
期刊：
The Journal of Chemical Physics
影响因子：
0
作者：
Curtis, Kevin;Adeyiga, Olajumoke;Suleiman, Olabisi;Odoh, Samuel O.
通讯作者：
Odoh, Samuel O.

Time-Dependent Density Functional Theory Study of Copper(II) Oxo Active Sites for Methane-to-Methanol Conversion in Zeolites

DOI：
10.1021/acs.inorgchem.0c03279
发表时间：
2021-01-05
期刊：
INORGANIC CHEMISTRY
影响因子：
4.6
作者：
Curtis, Kevin;Panthi, Dipak;Odoh, Samuel O.
通讯作者：
Odoh, Samuel O.

Performance of density functional theory for describing hetero‐metallic active‐site motifs for methane‐to‐methanol conversion in metal‐exchanged zeolites

密度泛函理论的性能用于描述金属交换沸石中甲烷向甲醇转化的异金属活性位点基序

DOI：
10.1002/jcc.25714
发表时间：
2018
期刊：
Journal of Computational Chemistry
影响因子：
3
作者：
Dandu, Naveen K.;Adeyiga, Olajumoke;Panthi, Dipak;Bird, Shaina A.;Odoh, Samuel O.
通讯作者：
Odoh, Samuel O.

Copper-Oxo Active Sites in the 8MR of Zeolite Mordenite: DFT Investigation of the Impact of Acid Sites on Methanol Yield and Selectivity