Collaborative Research: Rational Design of Alloys with Low-Melting-Point Metals for High-yield, Non-thermal Plasma-assisted Catalytic Production of Ammonia

合作研究：合理设计低熔点金属合金，用于高产率非热等离子体辅助催化生产氨

• 批准号: 2403970
• 负责人: Maria Carreon
• 金额: $ 20.66万
• 依托单位: University of Arkansas
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-10-01 至 2024-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2403970&HistoricalAwards=false
• 关键词: Collaborative; Research; Rational; Design; Alloys

Close to 2% of the world's energy is spent synthesizing ammonia by a chemical process called the Haber-Bosch process. Plasma catalysis is emerging as a promising alternative method for ammonia synthesis at moderate pressure and temperature, which allows it to rely on renewable energy resources that are more distributed and intermittent in nature. The goal of the proposed collaborative research project is to use computation and experiment to rationally design an alloy catalyst for a new plasma-assisted ammonia synthesis process that requires less energy. The research will also train students from underrepresented and minority groups and support the development and dissemination of educational materials on a general access website.The project will integrate experiments and simulations in a feedback loop that will culminate with the computational identification of a high-performance low melting point alloy that will be tested in catalytic experiments under an atmospheric plasma. The fundamental reaction mechanisms under plasma conditions will be elucidated by using kinetic Monte Carlo simulations. The research objectives of the project are: (1) Synthesize gallium alloys and evaluate kinetics of ammonia synthesis in a radio-frequency plasma reactor. (2) Determine recombination kinetics of H and N radicals from "plasma-on-plasma-off" experiments. (3) Calculate energetic descriptors for ammonia synthesis reaction steps under plasma conditions using Density Functional Theory. (4) Develop a kinetic Monte-Carlo model for ammonia formation using graph theoretical approach and cluster expansion. (5) Experimentally test a computationally identified alloy in a plasma reactor.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

通过称为Haber-Bosch工艺的化学过程，将近2％的世界能量用于合成氨。 血浆催化是一种在中等压力和温度下合成氨合成的有前途的替代方法，这使其可以依靠可再生能源资源在本质上更分布和间歇性。拟议的协作研究项目的目的是使用计算和实验来合理地设计合金催化剂，用于新的等离子体辅助氨合成过程，需要更少的能量。这项研究还将培训来自代表性不足和少数群体的学生，并支持一般访问网站上的教育材料的开发和传播。该项目将在反馈回路中整合实验和模拟，该实验和仿真将以高性能低熔点合金的计算识别在催化实验中测试的高强度低熔点合金，这将在大气质量下进行催化实验。 血浆条件下的基本反应机制将通过使用动力学蒙特卡洛模拟来阐明。该项目的研究目标是：（1）合成凝胶合金并评估射频等离子体反应器中氨合成动力学。 （2）确定从“等离子体启动”实验的H和N自由基的重组动力学。 （3）使用密度功能理论计算血浆条件下氨合成反应步骤的能量描述符。 （4）使用图理论方法和群集扩展开发一种动力学蒙特卡洛模型，以形成氨。 （5）在血浆反应器中测试了一种计算合金的实验测试。该奖项反映了NSF的法定任务，并且使用基金会的知识分子优点和更广泛的影响评估标准，被认为值得通过评估来获得支持。