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EAGER: Catalysis Fundamentals of Selective Hydrogenation of Aromatic Hydrocarbons

EAGER：芳烃选择性加氢的催化基础

基本信息

批准号：
2219872
负责人：
Simon Podkolzin
金额：
$ 20万
依托单位：
Stevens Institute of Technology
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2022
资助国家：
美国
起止时间：
2022-05-01 至 2024-12-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2219872&HistoricalAwards=false
关键词：
EAGER Catalysis Fundamentals Selective Hydrogenation

项目摘要

Catalysts speed up chemical reactions while promoting the selective conversion of feedstocks to desired products. Cyclic olefin compounds are a class of chemical compounds that are used widely in the chemical, pharmaceutical, and food industries. Their current manufacture, however, relies on inefficient catalysts and multistep processes that produce unwanted by-products, including hazardous and environmentally-unfriendly chemicals. Moreover, current feedstocks primarily consist of aromatic hydrocarbons derived from fossil sources. The project addresses the need for better fundamental understanding of the catalytic chemistry associated with cycloolefin manufacture. The fundamental insights will support development of models capable of predicting catalyst formulations and process conditions tuned to produce high yields of targeted products in energy-efficient single-step reactions. The models will be extended to biomass and other renewable feedstocks to enhance green chemistry and energy sustainability. Fundamental relationships between the structure of transition-metal catalysts and reactivity of aromatic hydrocarbons will be established at the molecular level via an integrated experimental-theoretical study focusing on single-step selective hydrogenation of hydrocarbons (containing one aromatic ring) to cycloolefins. Selective hydrogenation of tetralin to octalin will be used as a model reaction. Initial experiments will focus on previously identified promising catalysts consisting of supported Pd-Pt and Ni-Sn nanoparticles. Additional catalyst formulations will be selected based on the initial results. Experimental studies will provide information for the development of calibrated molecular models, which in turn will provide a better interpretation of the experimental results, and guide the selection of follow-up experiments to further improve the models in an iterative cycle. The study will synergistically and iteratively combine: (1) kinetic reaction measurements at steady-state and transient conditions, (2) in situ Raman and infrared vibrational spectroscopic measurements and (3) quantum-chemical calculations for interpretation of vibrational spectra, and transition state calculations for identification of reaction mechanisms. Elements of reaction engineering will be incorporated through kinetic models developed from data obtained over a range of temperature, reactant partial pressure, and reaction-time data. In addition to the technical aspects, the project will enable students to master critical skills needed to compete and contribute successfully in the international economy of the 21st century, particularly in the vital fields of sustainable chemical production and nanotechnology. The research team will also support undergraduate and K-12 educational outreach programs at the investigator’s institution.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.

催化剂加速化学反应，同时促进原料向所需产物的选择性转化。环烯烃化合物是一类广泛应用于化工、制药和食品工业的化合物。然而，它们目前的生产依赖于低效的催化剂和多步工艺，这些工艺会产生不需要的副产品，包括危险和对环境不友好的化学品。此外，目前的原料主要由源自化石来源的芳族烃组成。该项目解决了需要更好地了解与环烯烃制造相关的催化化学。这些基本见解将支持开发能够预测催化剂配方和工艺条件的模型，以在节能的单步反应中生产高产率的目标产品。这些模型将扩展到生物质和其他可再生原料，以提高绿色化学和能源的可持续性。通过对含一个芳环的烃类一步选择加氢反应的实验-理论研究，在分子水平上建立了过渡金属催化剂结构与芳烃反应活性之间的基本关系。将四氢萘选择性氢化为八氢萘用作模型反应。最初的实验将集中在以前确定的有前途的催化剂组成的负载Pd-Pt和Ni-Sn纳米粒子。将根据初步结果选择其他催化剂配方。实验研究将为校准分子模型的开发提供信息，这反过来又将为实验结果提供更好的解释，并指导后续实验的选择，以在迭代周期中进一步改进模型。该研究将协同和迭代地联合收割机结合：（1）在稳态和瞬态条件下的动力学反应测量，（2）原位拉曼和红外振动光谱测量和（3）用于解释振动光谱的量子化学计算，以及用于识别反应机理的过渡态计算。反应工程的元素将被纳入通过动力学模型从一系列的温度，反应物分压和反应时间数据获得的数据。除了技术方面，该项目还将使学生掌握在21世纪世纪的国际经济中成功竞争和贡献所需的关键技能，特别是在可持续化学生产和纳米技术的重要领域。该研究团队还将支持研究机构的本科生和K-12教育推广计划。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标准进行评估，被认为值得支持。