DFT-based Design and Experimental Testing of Catalytic Metallic Membranes for Selective N2-

基于 DFT 的选择性 N2- 催化金属膜设计和实验测试

• 批准号: 1263991
• 负责人: Jennifer Wilcox
• 金额: $ 32.5万
• 依托单位: Stanford University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-08-15 至 2016-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1263991&HistoricalAwards=false
• 关键词: DFT; based; Design; Experimental; Testing

Technical ImpactsThe current world population is just above 7 billion, of which 3-3.5 billion would not exist without the ammonia synthesis process. However, this process constitutes approximately 2.5% of the world's energy consumption. The United Nations estimate that world population is forecasted to reach 10 billion by the end of the century, which will inevitably lead to further reliance on the world's limited energy resources to produce ammonia fertilizer. There will be a corresponding increase in CO2 emissions, since the energy will likely be sourced from hydrocarbon oxidation. Replacement of this process technology with an improved process has been identified as one of the highest priorities in the recently published Technology Roadmap for Energy and GHG Reductions in the Chemical Industry (IEA, ICCA and Dechema, 2013). This award made jointly from the National Science Foundation Catalysis & Biocatalysis Program and the Chemical & Biological Separations Program is made to Professor Jennifer Wilcox of Stanford University to investigate an alternative strategy for ammonia synthesis with significantly reduced energy requirements. The technology involves the design and testing of a catalytic membrane reactor that will be used to dissociate N2 from the feed stream (front side of the membrane), leading to atomic N transport through the bulk crystal structure of the metallic membrane. In the permeate stream (backside of the membrane), H2 will be used as a sweep gas, ideally resulting in N-H coupling reactions and subsequent ammonia synthesis. This technology allows for the Earth-abundant elements such as vanadium and niobium (and not precious metals) to be used as the primary metals for nitrogen dissociation and transport. Wilcox has demonstrated preliminary data for some of the separations and reactions through an earlier NSF EAGER project. The remaining large technical risk is in devising the membrane and reactor system which performs the separations and catalyzes all the reactions together at a useful rate. Broader Impacts Broader impacts of the results of the proposed work are many. This technology offers a route to carry out the ammonia synthesis process at atmospheric pressures, adding huge savings to the agricultural chemical industry. Fertilizers are one of the most important factors in securing sufficient global food production. Demand is guaranteed to increase, as it is directly proportional to world population increase. Through the application of selective-N2 membrane technology, ammonia could be produced at a lower energy cost than the traditional high-pressure Haber-Bosch process. In addition to the science- and technology-based broader impacts, the PI plans to incorporate results from this research into a Carbon Capture course she developed in the Energy Resources Engineering department at Stanford University. Wilcox serves as a female role model for women in science, exhibited by the high number of female undergraduate and graduate students she has mentored. The exciting potential in this project should serve as a further attraction to increase females in engineering disciplines. Further dissemination of the results of the work will take place through the PI?s participation in the summer school program, Research Experience for Carbon Sequestration, which is supported by the Office of Fossil Energy of DOE and hosted annually by Southern Company. The summer school provides students with hands-on experience regarding CO2 capture and storage, with additional hosts including Alabama Power and the National Carbon Capture Center, which supports the testing of early capture technologies at the pilot scale. The PI will present findings through a course offered in the summer school program each year throughout the duration of the award.

技术影响当前的世界人口略高于70亿，其中3-35亿不存在，如果没有氨合成过程。但是，这个过程约占世界能源消耗的2.5％。联合国估计，到本世纪末，世界人口预计将达到100亿，这将不可避免地会进一步依赖世界上有限的能源来生产氨肥料。二氧化碳排放量将会增加，因为能量可能来自碳氢化合物氧化。在最近发表的化学工业中最近发表的技术路线图中，用改进的过程替换该过程技术已被确定为最高优先事项之一（IEA，ICCA和Dehema，2013年）。该奖项由美国国家科学基金会催化与生物催化计划共同颁发，并向斯坦福大学的詹妮弗·威尔科克斯教授颁布了化学与生物分离计划，以调查一项针对氨合成的替代策略，其能源需求大大减少。该技术涉及催化膜反应器的设计和测试，该催化膜反应器将用于从进料流中解离N2（膜的前侧），从而导致原子N通过金属膜的大块晶体结构。在渗透的流（膜的背面）中，H2将用作扫描气体，理想情况下导致N-H偶联反应和随后的氨合成。这项技术允许将土壤丰富的元素（例如钒和niobium（而不是贵金属））用作氮离解和运输的主要金属。 Wilcox通过早期的NSF急切项目展示了一些分离和反应的初步数据。其余的大技术风险在于设计膜和反应堆系统，该系统以有用的速度进行分离并将所有反应催化在一起。拟议工作结果的更广泛的影响更大。这项技术提供了在大气压力下进行氨合成过程的途径，为农业化学工业增加了巨大的节省。肥料是确保足够全球粮食生产的最重要因素之一。需求可以保证增加，因为它与世界人口的增加成正比。通过使用选择性N2膜技术，可以比传统的高压Haber-Bosch工艺以低的能源成本生产氨。除了基于科学和技术的广泛影响外，PI计划将这项研究的结果纳入她在斯坦福大学能源资源工程系中开发的碳捕获课程中。威尔科克斯（Wilcox）是科学女性的女性榜样，由她所指导的女性本科生和研究生众多。该项目的令人兴奋的潜力应该是增加工程学科女性的进一步吸引力。这项工作结果的进一步传播将通过PI参与暑期学校计划，碳固存的研究经验，该研究经验得到了DOE化石能源办公室的支持，并每年由南方公司主持。暑期学校为学生提供了有关二氧化碳捕获和存储的动手经验，其中包括阿拉巴马州电力在内的其他主机和国家碳捕获中心，该中心支持试点规模的早期捕获技术测试。 PI将在整个奖项期间每年通过暑期学校计划提供的课程介绍发现。