Evaluation of Novel Routes for NOx Formation in Remote Regions.
Evaluation of Novel Routes for NOx Formation in Remote Regions.
复制标题
偏远地区氮氧化物生成新途径的评估。
DOI：
10.1021/acs.est.6b06441
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发表时间：
2017-06
影响因子：
11.4
通讯作者：
C. Ye;D. Heard;L. Whalley
中科院分区：
文献类型：
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作者：
C. Ye;D. Heard;L. Whalley
氮氧化物（NOx）的光化学循环产生对流层臭氧（O3），传统上认为NOx是直接排放的。目前的全球模型无法准确计算NOx水平，同时，在低NOx制度（几个pptv或几十个pptv）全球范围内进行直接NOx测量的困难，引入了很大的不确定性的O3形成的建模。在这里，我们使用近明确的主化学机制（MCM v3.2）在一个0D箱模型框架内，描述的化学氮氧化物和O3在遥远的海洋边界层在佛得角。我们探讨了最近发现的氮氧化物回收途径，即颗粒硝酸盐的光解，氮氧化物丰度和O3形成的建模的影响。该模型被约束到观察长寿的物种，气象参数和光解频率。只有一个模型与这种新的氮氧化物再循环路线再现的气态亚硝酸，NO和NO2的模型和测量不确定性内的水平。由NO氧化形成O3的效率比以前认为的高几倍。这项研究强调了需要在未来的模型O3和颗粒硝酸盐的光解速率，以量化在可变的大气条件下的颗粒硝酸盐的光解。
Photochemical cycling of nitrogen oxides (NOx) produces tropospheric ozone (O3), and NOx is traditionally considered to be directly emitted. The inability of current global models to accurately calculate NOx levels, and concurrently, difficulties in performing direct NOx measurements in low-NOx regimes (several pptv or several tens of pptv) globally introduce a large uncertainty in the modeling of O3 formation. Here, we use the near-explicit Master Chemical Mechanism (MCM v3.2) within a 0D box-model framework, to describe the chemistry of NOx and O3 in the remote marine boundary layer at Cape Verde. We explore the impact of a recently discovered NOx recycling route, namely photolysis of particulate nitrate, on the modeling of NOx abundance and O3 formation. The model is constrained to observations of long-lived species, meteorological parameters, and photolysis frequencies. Only a model with this novel NOx recycling route reproduces levels of gaseous nitrous acid, NO, and NO2 within the model and measurement uncertainty. O3 formation from NO oxidation is several times more efficient than previously considered. This study highlights the need for the inclusion of particulate nitrate photolysis in future models for O3 and for the photolysis rate of particulate nitrate to be quantified under variable atmospheric conditions.