Université de Bordeaux, Institut des Sciences Moléculaires, F-33400 Talence, France.
Phys Chem Chem Phys. 2018 Jun 27;20(25):17442-17447. doi: 10.1039/c8cp02851f.
The gas-phase reaction of metastable atomic nitrogen N(2D) with nitric oxide has been investigated over the 296-50 K temperature range using a supersonic flow reactor. As N(2D) could not be produced photolytically in the present work, these excited state atoms were generated instead through the C(3P) + NO → N(2D) + CO reaction while C(3P) atoms were created in situ by the 266 nm pulsed laser photolysis of CBr4 precursor molecules. The kinetics of N(2D) atoms were followed on-resonance by vacuum ultraviolet laser induced fluorescence at 116.7 nm. The measured rate constants for the N(2D) + NO reaction are in excellent agreement with most of the earlier work at room temperature and represent the only available kinetic data for this process below 296 K. The rate constants are seen to increase slightly as the temperature falls to 100 K with a more substantial increase at even lower temperature; a finding which is not reproduced by theoretical work. The prospects for using this chemical source of N(2D) atoms in future studies of a wide range of N(2D) atom reactions are discussed.
使用超声速流反应器，在 296-50 K 的温度范围内研究了亚稳态氮原子 N(2D)与一氧化氮的气相反应。由于在本工作中不能光解产生 N(2D)，因此通过 C(3P) + NO → N(2D) + CO 反应产生这些激发态原子，而 C(3P)原子则通过 CBr4 前体分子的 266nm 脉冲激光光解原位生成。通过在 116.7nm 处的真空紫外激光诱导荧光，在共振条件下跟踪 N(2D)原子的动力学。所测量的 N(2D) + NO 反应的速率常数与室温下的大多数早期工作非常吻合，并且代表了该过程在 296K 以下唯一可用的动力学数据。随着温度降至 100K，速率常数略有增加，而在更低的温度下则有更大的增加；这一发现与理论工作不符。讨论了在未来研究中使用这种 N(2D)原子化学源的前景，研究范围广泛的 N(2D)原子反应。
