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: 1764116
• 负责人: Jeff White
• 金额: $ 24万
• 依托单位: Oklahoma State University
• 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 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764116&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. Dr. White of Oklahoma State University and Drs. Resasco, Crossley, and Wang of the University of Oklahoma 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.

需要强大的催化剂将原材料转化为有用的化学品，这对于开发更灵活和更低能源密集型的工艺至关重要。还需要能够使用各种来源的原材料，从石油到植物生物质再到再生塑料。催化剂需要能够在实际的反应条件下发挥作用，例如在存在污染物的情况下。许多催化剂已成功地用于工业过程，但需要高温和无湿的条件。俄克拉何马州立大学的怀特博士。俄克拉何马大学的Resasco、Crossley和Wang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环境下有效工作的新催化剂和新反应。了解水如何与催化剂和原料相互作用是实现这些目标所必需的。通过追求这些研究目标，该团队正在培养各级大学的学生。这使得本科生、研究生和代表性不足的群体能够成为国家STEM（科学、技术、工程和数学）基础设施的积极贡献者。该团队正在使用全州媒体来提高人们对基础催化研究如何影响经济上重要的行业的认识，无论是现在还是未来。在化学部化学催化项目的资助下，俄克拉何马州立大学和俄克拉何马大学的一个合作团队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。Drs。White、Resasco和Crossley从事沸石合成、沸石合成后改性、原位核磁共振光谱测量和不同温度和压力下的反应器研究，以确定催化剂结构对气相和液相水的反应。王博士提供DFT（密度泛函理论）和MD（分子动力学）计算来帮助团队阐明可能的反应途径。从传统石油来源衍生的非极性碳氢化合物以及从生物质衍生的含氧分子的转化都在研究中。也在调查的是小群体高度活跃的缺陷的作用。该团队正在通过每个校园的项目推进STEM学科中代表性不足的群体的纳入，并通过大学和州一级的公共媒体提高公众对催化益处的认识。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。

项目成果

Interaction of water with zeolites: a review

• DOI: 10.1080/01614940.2021.1948301
• 发表时间: 2021-04
• 期刊: Catalysis Reviews
• 作者: D. Resasco;S. Crossley;Bin Wang;Jeffery L. White

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