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

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、能源密集度更低的工艺至关重要。还需要有能力使用从石油到植物生物质再到回收塑料等各种来源的原材料。催化剂需要能够在现实的反应条件下发挥作用，例如在污染物存在的情况下。许多催化剂已经成功地用于工业过程，但需要高温和无湿条件。俄克拉荷马州立大学的怀特博士和俄克拉荷马大学的雷萨斯科博士、克罗斯利博士和王博士正在积极合作，将合成、测试和计算机模拟相结合，以帮助确定在较低温度和有水分的情况下将有效工作的新催化剂和新反应。要实现这些目标，需要了解水如何与催化剂和原料相互作用。通过追求这些研究目标，该团队正在对所有大学级别的学生进行培训。这使得本科生、研究生和代表性不足的群体能够为国家STEM(科学、技术、工程和数学)基础设施做出积极贡献。该团队正在利用全州范围的媒体提高人们对基础催化研究如何影响经济重要行业的认识，无论是现在还是未来。在化学部化学催化计划的资助下，来自俄克拉荷马州立大学和俄克拉荷马大学的一个合作小组正在使用一种跨学科的合成、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。White、Resasco和Crossley博士从事沸石的量身定制合成、沸石的合成后修饰、原位核磁共振光谱测量以及在不同温度和压力下的反应器研究，以确定催化剂结构对气相和液态水的反应。王博士正在提供密度泛函理论(DFT)和分子动力学(MD)计算，以帮助团队阐明可能的反应路径。来自传统石油来源的非极性碳氢化合物以及来自生物质来源的含氧分子的转化正在调查中。还在调查的是小种群高度活跃的作用？有缺陷吗？在没有水和存在水的情况下的催化站点该团队正在通过每个校园的计划推动将未被充分代表的群体纳入STEM学科，并通过大学和州一级的公共媒体提高公众对催化的好处的认识。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

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.