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First-Principles Design of Coke-Resistant Dehydrogenation Catalysts for Valorization of Light Hydrocarbon Feedstocks

用于轻质烃原料增值的抗焦脱氢催化剂的第一性原理设计

基本信息

批准号：
1705746
负责人：
Fuat Celik
金额：
$ 30万
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：
2017
资助国家：
美国
起止时间：
2017-09-01 至 2021-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1705746&HistoricalAwards=false
关键词：
First Principles Design Coke Resistant

项目摘要

The project will study the mechanism of poisoning of catalysts used to convert light hydrocarbon gases to higher value products. Specifically it will address coke formation - the process by which the hydrocarbons break down on the surface of the catalysts to form carbonaceous deposits that deactivate the catalyst. Mechanistic understanding will be derived from both theoretical predictions and experimental measurements, and will be used to predict, synthesize, and evaluate new catalyst formulations that are resistant to deactivation via coke formation. Poison-resistant dehydrogenation catalysts are needed to ensure effective utilization of the huge gas reserves associated with the Nation's shale resources. Efficient, durable, and economically attractive catalysts are essential for upgrading the light-gases to feedstocks of value to the energy and chemical sectors of the economy.The project will develop a fundamental understanding of the interaction between surface species and Pt-alloy dehydrogenation catalysts that give rise to their selectivity towards alkenes and for coke deposition during the high-temperature dehydrogenation of light alkanes. While the formation of the alkene has been studied, the mechanism of coke formation is unknown. Density Functional Theory (DFT) will be used to generate potential energy surfaces and kinetic activation barriers for the dissociation of alkanes to form carbonaceous surface species, thereby revealing how this mechanism is influenced by the electronic and geometric structure of the catalyst. Corresponding experimental studies will be carried out to understand the coking mechanism via analysis of the molecular fragments deposited on the catalyst surface. The insights from DFT and experimental characterization will be exploited to design new catalyst alloy structures and compositions with enhanced resistance to deactivation. Predicted designs will be experimentally validated by synthesizing the novel catalysts and testing their catalytic performance. Light alkanes, such as ethane and propane, produced as byproducts of hydrocarbon processing, and found naturally as minority components of natural gas, have little commercial value, and are sometime flared or burned only for their caloric value. Dehydrogenation of these hydrocarbons to their corresponding alkenes would produce higher-value intermediates especially attractive as chemical and polymer precursors. The results from this work will serve to build a diverse future chemical industry workforce through undergraduate chemical engineering curricula and recruiting of researchers from the diverse Rutgers undergraduate student body to contribute to the project.

该项目将研究用于将轻烃气体转化为高价值产品的催化剂中毒的机理。具体来说，它将解决焦炭的形成-碳氢化合物在催化剂表面分解形成使催化剂失活的碳质沉积物的过程。机理的理解将来自理论预测和实验测量，并将用于预测，合成和评估新的催化剂配方，耐失活通过焦炭形成。为了确保有效利用与国家页岩资源相关的巨大天然气储量，需要耐毒性脱氢催化剂。高效、耐用和经济上有吸引力的催化剂对于将轻质气体升级为能源和化学经济部门的有价值的原料至关重要。该项目将发展对表面物种和Pt合金脱氢催化剂之间相互作用的基本理解，这些相互作用导致其对烯烃的选择性和在轻质烷烃高温脱氢过程中的焦炭沉积。虽然已经研究了烯烃的形成，但是焦炭形成的机理是未知的。密度泛函理论（DFT）将被用来产生势能面和动力学活化障碍的烷烃的解离，形成碳质表面物种，从而揭示这种机制是如何影响的电子和几何结构的催化剂。通过对沉积在催化剂表面的分子碎片的分析，对结焦机理进行了相应的实验研究。 DFT和实验表征的见解将被用来设计新的催化剂合金结构和组合物，增强抗失活。预测的设计将通过合成新型催化剂和测试其催化性能进行实验验证。轻质烷烃，如乙烷和丙烷，作为烃加工的副产物产生，并且作为天然气的少数组分天然存在，几乎没有商业价值，并且有时仅为了它们的热值而燃烧或燃烧。将这些烃脱氢成其相应的烯烃将产生更高价值的中间体，作为化学品和聚合物前体特别有吸引力。这项工作的结果将有助于通过本科化学工程课程和从不同的罗格斯大学本科学生团体招募研究人员来为该项目做出贡献，从而建立一个多元化的未来化工行业劳动力队伍。