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，这是一种名为哈伯-博世工艺的化学工艺。等离子体催化是一种在中等压力和温度下合成氨的有前途的替代方法，这使得它可以依赖于在自然界中更分散和间歇性的可再生能源。提出的合作研究项目的目标是利用计算和实验合理地设计一种用于等离子体辅助氨合成的新工艺的合金催化剂，该工艺需要较少的能源。这项研究还将培训来自代表性不足和少数群体的学生，并支持在通用访问网站上开发和传播教育材料。该项目将在反馈回路中整合实验和模拟，最终通过计算识别出一种高性能低熔点合金，该合金将在大气等离子体下进行催化实验。等离子体条件下的基本反应机理将通过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)通过“等离子体-开-等离子体-关”实验确定H和N自由基的复合动力学。(3)用密度泛函理论计算了等离子体条件下氨合成反应步骤的能量描述。(4)利用图论方法和团簇展开方法建立了氨气生成的动力学蒙特卡罗模型。(5)在等离子体反应堆中对通过计算机识别的合金进行实验测试。这项裁决反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，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.