Collaborative Research: Understanding an Active and Beneficial Role for Water in Solid-Acid Catalyzed Hydrocarbon Chemistry

合作研究：了解水在固体酸催化碳氢化合物化学中的积极和有益的作用

• 批准号: 1764130
• 负责人: Steven Crossley
• 金额: $ 59.82万
• 依托单位: University of Oklahoma Norman Campus
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-07-01 至 2022-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764130&HistoricalAwards=false
• 关键词: Collaborative; Research; Understanding; Active; Beneficial

A need for robust catalysts to transform raw materials to useful chemicals is critical to developing more flexible and less energy intensive processes. The ability to use raw materials derived from various sources, ranging from petroleum to plant biomass to recycled plastics, is also needed. Catalysts need to be able to perform in realistic reaction conditions, such as in the presence of contaminants. Many catalysts have been successfully used in industrial processes but require high-temperature and moisture-free conditions. Drs. White, Resasco, Crossley, and Wang are engaged in an active collaboration that combines synthesis, testing, and computer simulations to help identify new catalysts and new reactions that will work efficiently at lower temperatures and in the presence of moisture. Understanding how water interacts with catalysts and feedstocks is required to meet these goals. Through pursuit of these research goals, the team is training students at all university levels. This is enabling undergraduate, graduate, and under-represented groups to be active contributors to the national STEM (science, technology, engineering, and mathematics) infrastructure. The team is using state-wide media to increase awareness of how fundamental catalysis research impacts economically important industries, both present and future. With funding from the Chemical Catalysis Program of the Chemistry Division, a collaborative team from Oklahoma State University and the University of Oklahoma is using an interdisciplinary synthesis, characterization, simulation, and reaction analysis approach to determine to whether or not water actively influences reactions in solid acid catalysts. Drs. White, Resasco, and Crossley, are engaged in tailored synthesis of zeolites, post-synthetic modifications of zeolites, in-situ spectroscopic NMR measurements, and reactor studies at varying temperature and pressure to determine how catalyst structure responds to the presence of both gas-phase and liquid-phase water. Dr. Wang is providing DFT (density functional theory) and MD (molecular dynamics) calculations to help the team elucidate probable reaction pathways. Conversion of both non-polar hydrocarbons derived for traditional petroleum sources as well as oxygenated molecules derived from biomass are under investigation. Also under investigation is the role of small populations of highly-active ?defect? catalytic sites in the absence and presence of water The team is advancing inclusion of under-represented groups in STEM disciplines through programs on each campus, and increasing public awareness of the benefit of catalysis through public media outlets at the university and state level.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.

需要强有力的催化剂将原材料转化为有用的化学品，这对于开发更灵活、能耗更低的工艺至关重要。 还需要有能力使用各种来源的原材料，从石油到植物生物质再到回收塑料。催化剂需要能够在现实的反应条件下，如在污染物的存在下进行。 许多催化剂已成功地用于工业过程，但需要高温和无水分的条件。 白色博士、Resasco博士、Crossley博士和Wang博士正在积极合作，将合成、测试和计算机模拟结合起来，以帮助确定在较低温度和潮湿条件下有效工作的新催化剂和新反应。 为了实现这些目标，需要了解水与催化剂和原料的相互作用。 通过追求这些研究目标，该团队正在培训所有大学级别的学生。这使得本科生，研究生和代表性不足的群体成为国家STEM（科学，技术，工程和数学）基础设施的积极贡献者。 该团队正在利用全州范围内的媒体来提高人们对基础催化研究如何影响当前和未来经济重要行业的认识。在化学部化学催化计划的资助下，来自俄克拉荷马州州立大学和俄克拉荷马州大学的一个合作小组正在使用跨学科的合成、表征、模拟和反应分析方法来确定水是否积极影响固体酸催化剂中的反应。 白色、Resasco和Crossley博士从事沸石的定制合成、沸石的合成后改性、原位光谱NMR测量以及在不同温度和压力下的反应器研究，以确定催化剂结构如何对气相和液相水的存在作出响应。 王博士提供DFT（密度泛函理论）和MD（分子动力学）计算，以帮助团队阐明可能的反应途径。 来自传统石油来源的非极性烃以及来自生物质的含氧分子的转化正在研究中。还在调查的是高活性的小群体的作用？背叛？该团队正在通过每个校园的项目，推动将代表性不足的群体纳入STEM学科，该奖项反映了NSF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进行评估，被认为值得支持的搜索.

项目成果

Structure and Catalytic Characterization of a Second Framework Al(IV) Site in Zeolite Catalysts Revealed by NMR at 35.2 T

• DOI: 10.1021/jacs.0c00590
• 发表时间: 2020-04-22
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Chen, Kuizhi;Horstmeier, Sarah;White, Jeffery L.
• 通讯作者: White, Jeffery L.

Quantifying the Influence of Water on the Mobility of Aluminum Species and Their Effects on Alkane Cracking in Zeolites

• DOI: 10.1021/acscatal.1c01138
• 发表时间: 2021-06
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: T. Pham;Vy T. Nguyen;Bin Wang;Jeffery L. White;S. Crossley

17 O Labeling Reveals Paired Active Sites in Zeolite Catalysts

17 O 标记揭示了沸石催化剂中的配对活性位点

• DOI: 10.1021/jacs.2c05332
• 发表时间: 2022
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Chen, Kuizhi;Zornes, Anya;Nguyen, Vy;Wang, Bin;Gan, Zhehong;Crossley, Steven P.;White, Jeffery L.
• 通讯作者: White, Jeffery L.