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.

技术影响目前世界人口略高于70亿，如果没有氨合成工艺，其中3- 35亿人口就不会存在。然而，这一过程约占世界能源消耗的2.5%。据联合国估计，到世纪末，世界人口将达到100亿，这将不可避免地导致进一步依赖世界有限的能源来生产氨肥。二氧化碳排放量将相应增加，因为能源可能来自碳氢化合物的氧化。最近出版的《化学工业能源和温室气体减排技术路线图》（国际能源机构、化学协会国际理事会和Dechema，2013年）将用改进的工艺取代这一工艺技术确定为最高优先事项之一。该奖项由美国国家科学基金会催化生物催化计划和化学生物分离计划联合颁发给斯坦福大学的Jennifer Wilcox教授，以研究一种显著降低能源需求的氨合成替代策略。该技术涉及催化膜反应器的设计和测试，该反应器将用于从进料流（膜的前侧）中解离N2，从而导致原子N通过金属膜的块状晶体结构传输。在渗透物流（膜的背面）中，H2将用作吹扫气体，理想地导致N-H偶联反应和随后的氨合成。这项技术允许地球上丰富的元素，如钒和铌（而不是贵金属）被用作氮分解和运输的主要金属。Wilcox通过早期的NSF EAGER项目展示了一些分离和反应的初步数据。剩下的大的技术风险在于设计膜和反应器系统，该系统以有用的速率进行分离并催化所有反应。拟议工作的结果将产生许多更广泛的影响。该技术提供了一种在大气压下进行氨合成工艺的途径，为农业化学工业节省了大量资金。肥料是确保全球粮食生产充足的最重要因素之一。需求肯定会增加，因为它与世界人口增长成正比。通过选择性N2膜技术的应用，可以以比传统高压哈伯-博世工艺更低的能源成本生产氨。除了基于科学和技术的更广泛的影响，PI计划将这项研究的结果纳入她在斯坦福大学能源工程系开发的碳捕获课程。威尔科克斯是女性在科学领域的女性榜样，她所指导的女性本科生和研究生人数众多。该项目令人兴奋的潜力应进一步吸引更多的女性进入工程学科。将通过PI进一步传播工作成果？参加暑期学校项目，碳封存研究经验，该项目由美国能源部化石能源办公室支持，每年由南方公司主办。暑期学校为学生提供有关二氧化碳捕获和储存的实践经验，其他主机包括亚拉巴马电力和国家碳捕获中心，支持在试点规模测试早期捕获技术。PI将在整个奖项期间每年通过暑期学校课程提供的课程展示调查结果。