Catalytic Partial Oxidation of Lower Alkanes

低级烷烃的催化部分氧化

• 批准号: 9412544
• 负责人: Umit Ozkan
• 金额: $ 33.67万
• 依托单位: Ohio State University Research Foundation -DO NOT USE
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1994
• 资助国家: 美国
• 起止时间: 1994-11-15 至 1999-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9412544&HistoricalAwards=false
• 关键词: Catalytic; Partial; Oxidation; Lower; Alkanes

ABSTRACT CTS-9412544 Umit Ozkan This is a fundamental study of the catalytic phenomena involved in the activation and partial oxidation of methane and ethane. The objectives include investigation of the natures of the active sites responsible for alkane activation and oxygen insertion on supported and unsupported vanadia and molybdena catalysts, control of selectivity on these sites by modifiers (both promoters and inhibitors) such as alkali metals, phosphorus, and halides, the roles of coreactants and additives on the reaction schemes, and the reaction networks responsible for partial oxidation of methane and ethane. Catalysts are characterized both before and after reaction using BET surface-area measurements, pore size distribution, X-ray diffraction, X-ray fluorescence, laser Raman spectroscopy, X-ray photoelectron spectroscopy, Auger electron spectroscopy, secondary-ion mass spectroscopy, and thermal analysis techniques. In - situ laser Raman characterization is combined with isotopic labelling to identify oxygen insertion sites. Steady- state and transient kinetic studies and isotopic labelling are used as mechanistic probes to examine the catalytic routes to partial and complete oxidation. Methane and ethane are readily available inexpensive feedstocks, and the conversion of methane to formaldehyde or methanol and ethane to ethylene or acetaldehyde has been a major objective of catalytic technology. These conversions are easy to achieve, but the fine control needed to isolate these products has been elusive; most processes produce mainly carbon monoxide and carbon dioxide which are formed both from competitive reaction pathways and from further oxidation of the indended products. Better understanding of the operative mechanisms will permit new control strategies to solve this classical problem.

摘要CTS-9412544 UMIT Ozkan这是对甲烷和乙烷激活和部分氧化涉及的催化现象的基本研究。 目的包括研究负责烷烃激活和氧气插入的活性位点的自然作用，并置于受支持和不受支持的瓦纳迪亚和钼催化剂上，通过修饰符（启动子和抑制剂）对这些站点的选择性控制，例如碱金属，磷酸盐和磷酸盐的反应，以及磷酸属性，以及磷酸化的反应，并构成均可分子，并构成均可分子，典型的摩尔和骨质，均可分子，均可菌落和均可菌落，均可分子，典型的摩尔菌，均可菌落和反应均匀的摩尔菌，均可及其层状，均可菌落和反应均可菌落和反应均匀的摩尔和均匀的摩尔和菌落的序列，均可菌落和典型的成分和均匀的摩尔和均匀的成分迹象。用于甲烷和乙烷的部分氧化。 使用BET表面面积测量值，孔径分布，X射线衍射，X射线荧光，激光拉曼光谱，X射线光电学光谱，螺旋螺旋式电子光谱，次级ION质谱和热分析技术来表征催化剂在反应前后的表征。 在 - 原位激光拉曼表征与同位素标记结合在一起，以识别氧气插入位点。 稳态和瞬态动力学研究和同位素标记用作检查部分和完全氧化的催化途径的机械探针。 甲烷和乙烷很容易获得廉价的原料，将甲烷转化为甲醛或甲醇和乙烷，或乙烷或乙醛或乙醛是催化技术的主要目标。 这些转换很容易实现，但是隔离这些产品所需的精细控制是难以捉摸的。大多数过程主要产生一氧化碳和二氧化碳，它们既由竞争反应途径，也是由会产物的进一步氧化而形成的。 更好地了解手术机制将允许新的控制策略解决这个经典问题。