GOALI: Atomic Tailoring of Catalyst Surfaces for High Selectivity: Partial Oxidation of Propane

目标：高选择性催化剂表面的原子定制：丙烷的部分氧化

• 批准号: 0432593
• 负责人: John Gleaves
• 金额: $ 30.27万
• 依托单位: Washington University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2004
• 资助国家: 美国
• 起止时间: 2004-09-01 至 2008-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0432593&HistoricalAwards=false
• 关键词: GOALI; Atomic; Tailoring; Catalyst; Surfaces

AbstractProposal Title: GOALI: Atomic Tailoring of Catalyst Surfaces for High Selectivity: Partial Oxidation of Propane Proposal Number: CTS-0432593Principal Investigator: John T. GleavesInstitution: Washington University Mixed metal oxides (MMO) are widely used as catalysts in the petroleum, chemical, environmental, and pharmaceutical industries. A controlling factor in catalyst performance is the concentration of oxygen and metal species in the MMO surface. Industrial MMO catalysts are prepared by bulk techniques, which provide limited control of surface properties. Samples with the same bulk crystal structure and composition can exhibit different performance when prepared by different routes. This difference may be attributed to a change in the surface concentration of one or more of the catalyst constituents. This GOALI research project will establish a new method of adding atoms to the surface of bulk catalytic materials while maintaining the same bulk composition, and charting the change in catalytic properties as the surface is heated or exposed to a reactant mixture. This new process, dubbed "atomic tailoring", will be used to develop highly selective and active catalysts for the partial oxidation of propane to acrylic acid. Atomic beam deposition, a technique used in surface science, has been adapted so that metal atoms (including those with high melting points) can be directly deposited on particles. After deposition, special vacuum transient response experiments (called TAP experiments) will be used to monitor catalytic properties as the modified material is heated and exposed to a reactant atmosphere.Improved catalysts for propane conversion to acrylic acid will allow propane to replace propene as a feedstock. The lower feedstock cost for propane, coupled with reduced capital afforded by a direct rather than two-step process, will lower production costs by 20-25%. The knowledge gained from fabricating more active and selective partial oxidation catalysts for propane will be applicable to other selective oxidation reactions, especially reactions of other alkanes. From a U.S. economic and environmental perspective, the development of new catalysts for alkane activation and selective oxidation to commercially useful products will deliver energy savings of up to 37 trillion BTUs/yr and will significantly reduce the generation of green-house gases. Published results from this study will also be useful to other researchers who are designing experiments to probe molecular level processes on complex catalytic surfaces. This GOALI program will introduce graduate and undergraduate students to exciting real-world problems that when solved will have a significant economic, social, and environmental impact. Students will work as part of a diverse team, and they will gain hands-on experience designing, building, and running complex experiments that define the state of the art. The program strongly encourages minority and female students to become involved in research while still encouraging all undergraduates to pursue advanced degrees. Graduate and undergraduate students will work with industrial researchers at an industrial laboratory and will have the opportunity to present their work at academic-industrial group meetings and at national scientific meetings.

摘要提案标题：目标：高选择性催化剂表面的原子修整：丙烷部分氧化提案编号：CTS-0432593主要研究者： John T. Glephon机构： 华盛顿大学混合金属氧化物（MMO）被广泛用作石油、化工、环境和制药工业的催化剂。 催化剂性能的控制因素是MMO表面中氧和金属物质的浓度。工业MMO催化剂通过本体技术制备，其提供有限的表面性质控制。具有相同体相晶体结构和组成的样品，当通过不同的路线制备时，可以表现出不同的性能。这种差异可归因于一种或多种催化剂组分的表面浓度的变化。 这个GOALI研究项目将建立一种新的方法，将原子添加到块状催化材料的表面，同时保持相同的块状成分，并绘制催化性能的变化，因为表面被加热或暴露于反应混合物。这种被称为“原子剪裁”的新工艺将用于开发丙烷部分氧化制丙烯酸的高选择性和活性催化剂。 原子束沉积是一种用于表面科学的技术，已经被改造成可以将金属原子（包括那些具有高熔点的金属原子）直接沉积在颗粒上。沉积后，将使用特殊的真空瞬态响应实验（称为TAP实验）来监测改性材料在加热和暴露于反应物气氛中时的催化性能。用于丙烷转化为丙烯酸的改进催化剂将允许丙烷取代丙烯作为原料。丙烷的原料成本较低，再加上直接而不是两步法提供的资本减少，将使生产成本降低20- 25%。本研究所获得的丙烷选择性部分氧化催化剂的制备方法，对其它烷烃的选择性氧化反应，特别是其它烷烃的选择性氧化反应具有一定的指导意义。从美国经济和环境的角度来看，开发用于烷烃活化和选择性氧化为商业上有用的产品的新催化剂将节省高达37万亿BTU/年的能源，并将显著减少温室气体的产生。 这项研究的结果也将有助于其他研究人员设计实验来探测复杂催化表面上的分子水平过程。该GOALI计划将向研究生和本科生介绍令人兴奋的现实问题，这些问题解决后将产生重大的经济，社会和环境影响。学生将作为一个多元化的团队的一部分工作，他们将获得实践经验，设计，建造和运行复杂的实验，定义了最先进的状态。该计划强烈鼓励少数民族和女性学生参与研究，同时仍然鼓励所有本科生追求更高的学位。研究生和本科生将在工业实验室与工业研究人员合作，并有机会在学术工业小组会议和国家科学会议上展示他们的工作。