CAREER: Environmentally Significant Reforming Reactions Studied Using a Novel Catalytic Shock Tube.

职业：使用新型催化激波管研究对环境具有重要意义的重整反应。

• 批准号: 1341133
• 负责人: Marco Castaldi
• 金额: $ 22.62万
• 依托单位: CUNY City College
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-01 至 2016-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1341133&HistoricalAwards=false
• 关键词: CAREER; Environmentally; Significant; Reforming; Reactions

0846330CastaldiThe proposed work uses an innovative technique to investigate the chemical kinetics and mechanisms of catalytic reactions by combining a high pressure shock tube normally used for homogeneous reaction analysis and adapting it to study heterogeneous reactions. This technique will resolve the mechanistic uncertainties that have evolved using conventional continuous flow techniques and through their resolution lead to potentially significant impacts on energy generation and the quality of the environment. The new technique incorporates a catalyzed short contact time (SCT) reactor substrate into a high pressure single pulse shock tube. The combination of a SCT reactor and shock tube enables the study, by detection of intermediates, of the mechanism of complex heterogeneous reactions over a catalyst for very well defined times and conditions in the absence of transport effects that plague conventional techniques. The mechanistic understanding arising from the unique conditions of the shock tube will facilitate a smooth transition in scale-up from the lab to industrial applications where high pressures are necessary for increased process throughput. One example of the mechanistic information that will be the focus of the proposed work is the resolution of the routes to synthesis gas (an alternate energy source) during the Catalytic Partial Oxidation (CPOX) of methane. One hypothesized route is through a partial oxidation step which must be terminated, for syn-gas production, before complete oxidation. This route can be established by detection of CO and H2 before CO2 formation. An alternative route is through complete oxidation to CO2 followed by secondary reforming to syn-gas which can be evaluated through measurements of the relative rates of the co-formation of CO2 and CO/H2. Another mechanistic problem to be addressed arises in the catalytic reforming of the green house gas CO2 with methane. Although the atmospheric pressure, water free mechanism of this process has been established its relevance to practical process conditions has not. Process conditions would probably require the use of steam to suppress carbon formation on the reforming catalysts and elevated pressure to increase throughput. A catalytic process operating at elevated pressure with water addition will almost certainly involve a different mechanism than the one already established. Detection and quantification of key oxygenated intermediates, such as methanol and formaldehyde, by the new technique of combining a SCT reactor with a high pressure single pulse shock tube will establish the mechanism and guide practical reactor design. Broader impacts and Societal Benefits 1) Elucidation of the mechanism of catalytic partial oxidation of methane to synthesis gas for its use as an alternative energy source in environmentally friendly processes. 2) Optimization of methane reforming of carbon dioxide potentially leading to the reduction of these greenhouse gases. 3) Development and evaluation of a novel short contact time reactor/single pulse shock tube methodology for studying catalytic reactions important to maintaining a clean living environment. 4) Development of catalytic methods at high pressures for increased process throughput. 5) Investigation of alternate catalysts for CPOX and CO2 reforming. 6) Education of graduate students in the cross disciplinary fields of catalytic chemistry, environmental science, high pressure shock tube experimentation and reaction engineering.

0846330 castaldithe提出的工作使用创新技术来研究通常用于均质反应分析的高压冲击管，研究催化反应的化学动力学和机制，并将其调整以研究异质反应。该技术将解决使用常规连续流技术进化的机械不确定性，并通过其解决方案导致对能源产生和环境质量的潜在显着影响。新技术将催化的短接触时间（SCT）反应器底物纳入高压单脉冲冲击管中。 SCT反应器和冲击管的组合可以通过检测中间体的研究，在催化剂上复杂的异质反应的机制，即在缺乏困扰常规技术的运输效应的情况下，在非常确定的时间和条件下进行了研究。电击管的独特条件产生的机械理解将有助于从实验室到工业应用的平稳过渡，在这些应用中，对于增加过程吞吐量需要高压力。所提出的工作重点的机理信息的一个例子是在甲烷的催化部分氧化（CPOX）期间的合成气（替代能源）的途径解决。一个假设的途径是通过部分氧化步骤，必须在完全氧化之前终止同时气体的产生。可以通过在CO2形成之前检测CO和H2来确定此途径。另一种途径是通过对CO2的完全氧化，然后进行二次改革，与Syn-Gas进行二次改革，可以通过测量CO2和CO/H2的共形成速率来评估。在用甲烷对温室气体二氧化碳二氧化碳的催化重整时，要解决的另一个机械问题。尽管大气压力，但该过程的无水机制与实际过程条件的相关性尚未建立。工艺条件可能需要使用蒸汽抑制在改革催化剂上的碳形成，并增加压力以增加吞吐量。在加含水的压力下运行的催化过程几乎肯定涉及与已经建立的机制不同的机制。通过将SCT反应器与高压单脉冲冲击管组合的新技术的检测和定量，例如甲醇和甲醛，例如甲醇和甲醛。更广泛的影响和社会益处1）阐明甲烷催化部分氧化与合成气体的机理，以用作环保过程中的替代能源。 2）优化二氧化碳的甲烷改革可能导致这些温室气体的减少。 3）新型短接触时间反应器/单脉冲电击管的开发和评估，用于研究对维持清洁生活环境很重要的催化反应。 4）在高压下开发催化方法，以增加过程吞吐量。 5）调查CPOX和CO2改革的替代催化剂。 6）在催化化学，环境科学，高压冲击管实验和反应工程的跨学科领域的研究生教育。