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

世界上近2%的能源用于合成氨，这是一种称为哈伯-博世工艺的化学过程。 等离子体催化正在成为一种有前途的替代方法，用于在中等压力和温度下合成氨，这使其能够依赖于可再生能源，这些能源在性质上更加分散和间歇。本合作研究项目的目的是通过计算和实验，合理设计一种用于新的等离子体辅助氨合成工艺的合金催化剂，该工艺需要更少的能量。该研究还将培训来自代表性不足和少数群体的学生，并支持在一个通用网站上编写和传播教育材料，该项目将把实验和模拟纳入一个反馈回路，最终将通过计算识别一种高性能低熔点合金，该合金将在大气等离子体下的催化实验中进行测试。 等离子体条件下的基本反应机制将通过使用动力学蒙特卡罗模拟来阐明。本项目的研究目标是：（1）在射频等离子体反应器中合成镓合金并评价氨合成动力学。(2)从“等离子体开-等离子体关”实验中确定H和N自由基的复合动力学。(3)使用密度泛函理论计算等离子体条件下氨合成反应步骤的能量描述符。(4)利用图论方法和团簇展开建立了氨生成的蒙特-卡罗动力学模型。(5)在等离子体反应器中对计算识别的合金进行实验测试。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估而被认为值得支持。

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.