Photochemical production and release of gaseous NO2 from nitrate-doped water ice

Boxe CS; Colussi AJ; Hoffmann MR; Murphy JG; Wooldridge PJ; Bertram TH; Cohen RC

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Photochemical production and release of gaseous NO2 from nitrate-doped water ice

机译：从硝酸盐掺杂的水冰中光化学产生并释放出气态NO2

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Temperature-programmed NO2 emissions from frozen aqueous NaNO3 solutions irradiated at 313 nm were monitored as function of nitrate concentration and heating rate, H, above -30 degrees C. Emissions increase nonmonotonically with temperature, displaying transitions suggestive of underlying metamorphic transformations. Thus, NO2 emissions surge at ca. -8 degrees C in frozen [NO3-] > 200 mu M samples warmed at H = 0.70 degrees C min(-1) under continuous irradiation, and also in the dark from samples that had been photolyzed at -30 degrees C. The amounts of NO2 released in individual thermograms, Sigma(N), increase less than linearly with [NO3-] or the duration of experiments, revealing the significant loss of photogenerated NO2. The actual Sigma(N) proportional to [NO3-](1/2) dependence (at constant H) is consistent with NO2 hydrolysis: 2NO(2) + (HO)-O-2 -> NO3- + NO2- + 2H(+), overtaking NO2 desorption, even below the eutectic point (-18 degrees C for aqueous NaNO3). The increasingly larger NO2 losses detected in longer experiments (at constant [NO3-]) are ascribed to secondary photolysis of trapped NO2. The relevance of present results to the interpretation of polar NO2 measurements is briefly analyzed.

机译：在-30 nm以上，监测了在313 nm下冷冻的NaNO3水溶液照射的程序升温NO2排放，它是硝酸盐浓度和加热速率H的函数。排放随温度非单调增加，显示出表明潜在的变质转变的过渡。因此，NO2排放大约在在连续照射下，在H = 0.70°C min（-1）下加热的[NO3-]> 200μM冷冻样品中，温度为-8摄氏度，在-30℃下光解的样品在黑暗中也是如此。在各个温度记录图中释放的NO2的总和（Sigma（N））随[NO3-]或实验持续时间的增加而线性减少，这表明光生NO2的大量损失。与[NO3-]（1/2）依赖性成正比的实际Sigma（N）（在恒定H下）与NO2水解一致：2NO（2）+（HO）-O-2-> NO3- + NO2- + 2H （+），甚至在低于共晶点（NaNO3水溶液为-18摄氏度）以下时，仍能超过NO2解吸。在较长时间的实验中（以[NO3-]不变）检测到的越来越多的NO2损失归因于捕获的NO2的二次光解。简要分析了当前结果与解释极性NO2测量值的相关性。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2005年第38期|共6页
作者
Boxe CS; Colussi AJ; Hoffmann MR; Murphy JG; Wooldridge PJ; Bertram TH; Cohen RC;
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正文语种 eng
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DEPENDENT SOLUTE REDISTRIBUTION; AQUEOUS-SOLUTION; QUANTUM YIELDS; NITROGEN-DIOXIDE; PHASE BOUNDARY; ANTARCTIC ICE; SNOW; PHOTOLYSIS; GREENLAND; NITRITE;

机译：依赖的溶质再分配;水溶液;季铵盐;一氧化二氮;相界;南极冰;雪;光解作用;格陵兰;亚硝酸盐;

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Photochemical production and release of gaseous NO2 from nitrate-doped water ice

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