Abstract An improved understanding of NOx formation at high pressures would be of considerable utility to efforts to develop advanced combustion devices. A combination of theoretical and modeling studies are implemented in an effort to improve the accuracy of models for the prompt NO process, which is the dominant source of NO under many conditions, and to improve our understanding of the role of this process at high pressures. The theoretical effort implements state-of-the-art treatments of NCN thermochemistry, the interrelated CH + N2 and NCN + H kinetics, and the kinetics of the NCN + OH reaction. For both reaction systems, we implement high level ab initio transition state theory based master equation simulations paying particular attention to the role of stabilization processes. For the NCN + H kinetics we include a treatment of inter-system crossing. The modeling effort focuses on exploring the role of pressure and prompt NO for premixed laminar flames at pressures ranging from 1 to 15 atm, via a comparison with the available experimental data. Additional simulations at higher pressures further explore the mechanistic changes at the pressures of relevance to applied combustion devices (e.g., 100 atm).

中文翻译：

---

与高压下瞬发一氧化氮形成相关的理论和建模

摘要 对高压下 NOx 形成的更好理解对于开发先进燃烧装置的努力具有重要意义。理论和建模研究相结合，旨在提高瞬发 NO 过程模型的准确性，这是许多条件下 NO 的主要来源，并提高我们对该过程在高压下的作用的理解。理论工作实现了 NCN 热化学、相互关联的 CH + N2 和 NCN + H 动力学以及 NCN + OH 反应动力学的最先进处理方法。对于这两个反应系统，我们实施了基于主方程模拟的高级从头过渡态理论，特别注意稳定过程的作用。对于 NCN + H 动力学，我们包括系统间交叉的处理。建模工作的重点是通过与可用实验数据的比较，探索压力和提示 NO 在压力范围为 1 到 15 个大气压下的预混层流火焰中的作用。更高压力下的额外模拟进一步探索了与应用的燃烧装置相关的压力（例如，100 个大气压）下的机械变化。