Formation of Nitrogen Oxides by Nanosecond Pulsed Plasma Discharges in Gas–Liquid Reactors
Formation of Nitrogen Oxides by Nanosecond Pulsed Plasma Discharges in Gas–Liquid Reactors
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DOI：
10.1007/s11090-019-09981-w
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发表时间：
2019-05
影响因子：
3.6
通讯作者：
R. Wandell;Huihui Wang;R. Bulusu;Rachel O. Gallan;B. Locke
中科院分区：
文献类型：
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作者：
R. Wandell;Huihui Wang;R. Bulusu;Rachel O. Gallan;B. Locke
利用纳秒脉冲电源的气液膜流动反应器，以Ar/N2混合物(气相)和去离子水(液体相)为原料制备氮氧化物。对气相和液相中发现的稳定产物进行了化学分析，并对液相样品进行了化学猝灭，以消除等离子体后反应。用傅里叶变换红外光谱和离子色谱分别测定了气相和液相中大量的NO和NO2。氮氧化物的生成速率随氮气浓度的增加而显着增加，而过氧化氢的生成量略有下降。等离子体的气体温度约为525K，不受氮气浓度的影响，电子密度在纯Ar中为1 × 1017 cm−3，在28%氮气中为5.5 × 1017 cm−3。通过加入CO作为气相自由基清除剂，评价了TH在反应过程中的作用，表明TH对气相NO和NO2转化为水溶态是必不可少的。相反，来自水的原子氧很可能是产生NO和NO2的原因。用氮气/氧气/Ar混合气体和空气进行的实验表明，由于额外生成的活性氧物种，NO2的产生显著增加。在最有效的情况下产生的所有氮氧化物的总能量产量为50EV/分子。
A gas–liquid-film flow reactor with a nanosecond pulsed power supply was utilized to produce nitrogen oxides from Ar/N2mixtures (gas phase) and deionized water (liquid phase). Chemical analysis of the stable products found in both the gas and liquid phases was performed and chemical quenching was incorporated for the liquid phase samples in order to eliminate post plasma reactions. Significant amounts of NO and NO2in the gas phase andandin the liquid phase were determined using FTIR spectroscopy and ion chromatography, respectively. The production rate of all nitrogen oxides produced increased significantly with N2concentration while H2O2formation decreased slightly. The gas temperature of the plasma was approximately 525 K and was unaffected by N2concentration while the electron density ranged from 1 × 1017cm−3in pure Ar to 5.5 × 1017cm−3in 28% N2. The role of thein the reaction pathway was assessed by adding CO as a gas phase radical scavenger showing thatis essential for conversion of the gas phase NO and NO2into water solubleand. Conversely, atomic oxygen originating from water is likely responsible for NO and NO2generation. Experiments with N2/O2/Ar mixtures and air showed a significant increase in NO2production caused by the additional generation of reactive oxygen species. An overall energy yield for all nitrogen oxides produced in the most efficient case was 50 eV/molecule.