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CAREER:Revolutionizing Propylene Production via Oxidative Dehydrogenation and CO2 Dissociation in Tandem

事业：通过串联氧化脱氢和二氧化碳解离彻底改变丙烯生产

基本信息

批准号：
1751683
负责人：
George Tsilomelekis
金额：
$ 50万
依托单位：
Rutgers University New Brunswick
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：
2018-06-01 至 2024-05-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1751683&HistoricalAwards=false
关键词：
CAREER Revolutionizing Propylene Production via

项目摘要

The development of catalytic routes for converting lower alkanes to olefins is a challenging problem with high potential payoff due to the vast shale gas resources that have recently become available. The overarching goal of this project is to revolutionize propylene production from alkanes through an innovative tandem catalytic reaction scheme that improves overall conversion and selectivity. The project is based on a potentially transformative approach where new paradigms in reaction mechanisms guide catalyst synthesis. A hierarchical framework will be developed for rational design and characterization of catalysts with significant potential broader impact in the energy, petrochemical and chemical sectors of the US industry.The main objective of this project is to develop a new class of bifunctional catalysts based on sub-stoichiometric nanophase metal oxides that will work in a tandem reaction scheme, where oxidative dehydrogenation of alkanes and carbon dioxide reduction, via dissociative adsorption, will occur simultaneously without producing syngas. The proposed novel tandem reaction scheme has the potential to intensify on-purpose propylene production by preventing side reactions, such as coke formation, and further aromatization of propylene. A new facile synthesis method for producing oxygen-deficient anatase nanosheet catalysts is proposed by utilizing highly amorphous solubilized cellulose as a sacrificial template. The proposed experimental framework is based on optical reactor prototyping and Operando spectroscopy, where the molecular structure and reactivity of the metal oxide catalysts are studied simultaneously in a single optical cell by time- and spatially-resolved Raman spectroscopy under real working conditions. Integration of research and education is focused towards modernizing the chemical reaction engineering curriculum with teaching modules on Operando spectroscopy. Outreach efforts are aimed at engaging K-12 students, including underrepresented minorities, by developing a freeware computer game that teaches principles of molecular symmetry and spectroscopy.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.

由于最近获得了大量的页岩气资源，开发将低碳烷烃转化为烯烃的催化路线是一个具有高潜在回报的具有挑战性的问题。该项目的总体目标是通过一种创新的串联催化反应方案来提高整体转化率和选择性，从而彻底改变烷烃生产丙烯的方式。该项目基于一种潜在的变革性方法，即反应机理中的新范式指导催化剂合成。该项目的主要目标是开发一种基于亚化学计量比纳米金属氧化物的新型双功能催化剂，该催化剂将以串联反应模式工作，其中烷烃的氧化脱氢和二氧化碳的还原将通过解离吸附同时进行，而不会产生合成气。建议的新型串联反应方案有可能通过防止副反应，如结焦和丙烯的进一步芳构化，来强化目的丙烯的生产。提出了一种以高度无定形可溶纤维素为牺牲模板制备缺氧型锐钛矿型纳米片状催化剂的新方法。所提出的实验框架基于光学反应器原型和操纵面光谱，在单个光池中通过时间和空间分辨拉曼光谱同时研究了真实工作条件下金属氧化物催化剂的分子结构和反应活性。研究与教育相结合的重点是使化学反应工程课程现代化，并提供关于操作光谱学的教学模块。推广活动的目的是通过开发一款教授分子对称原理和光谱学原理的免费电脑游戏，吸引K-12年级的学生，包括未被充分代表的少数族裔。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。