华北地区有机涂层下五氧化二氮非均相过程参数化方案评价

IF 3.7 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment Pub Date : 2025-06-04 DOI:10.1016/j.atmosenv.2025.121335

Yu Qu , Juan Yang , Yitian Guo , Yong Chen , Xingang Liu , Hui Chen , Haiyan Ran , Jingwei Zhang , Ying Li , Junling An

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引用次数: 0

摘要

五氧化二氮（N2O5）的非均相反应是夜间硝酸盐形成的重要途径，其参数化非常复杂，特别是在有机涂层存在（考虑相变）的情况下。本研究将无机核(Davis08) -有机壳（Gaston14和Riemer09）的N2O5水解参数化方案整合到化学天气研究与预报模型中，讨论了有机涂层对华北地区粒径分解N2O5吸收系数和硝酸盐的模拟差异，这些差异尚未有报道。3种粒径N2O5吸收系数均存在显著的时空差异，其中粒径2 （156 ~ 625 nm）最大。由于相对湿度（RH）的变化，东部沿海和相对清洁地区的数值普遍大于内陆和污染地区，而在硝酸盐占主导地位的地区则受到抑制。Riemer09方案与SOA（二次有机气溶胶）包层厚度（l/Rp）有关，在l/Rp≥0.08、γD（无机核心吸收系数）≥1 × 10−2的区域，产生至少2 μg/m3的硝酸盐抑制作用。方案Gaston14考虑了环境RH和SOA阶段的影响；在相对湿度大于70%的区域，方案Gaston14模拟的覆膜效果相对较小；低RH （< 40%）和低O:C比（<0.48）同时存在时，方案Gaston14具有显著的包覆效应，其模拟的硝酸盐比方案Riemer09的模拟低~ 4 μg/m3。两种涂覆方案呈现出相似的垂直趋势，在~ 240m高度，污染区域2号粒径桶中不均匀产生的硝酸盐最大差异为15%。方案Gaston14在复杂气象和气溶胶条件下表现出更大的优势。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Evaluating parameterization schemes of dinitrogen pentoxide heterogeneous processes in the presence of organic coatings for size-resolved nitrate simulations over North China

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Evaluating parameterization schemes of dinitrogen pentoxide heterogeneous processes in the presence of organic coatings for size-resolved nitrate simulations over North China

The heterogeneous reaction of dinitrogen pentoxide (N₂O₅) is an important pathway for the nighttime formation of nitrate and its parameterization especially in the presence of organic coatings (considering phase changes) is complicated. In this study, an updated combination of inorganic core (Davis08) - organic shell (Gaston14 and Riemer09) parameterization schemes for N₂O₅ hydrolysis was embedded into the Weather Research and Forecasting model with Chemistry to discuss the simulated differences of and organic coating impacts on size-resolved N₂O₅ uptake coefficients and nitrate in North China, which have not been reported. All the three size-resolved N₂O₅ uptake coefficients had significant spatiotemporal variations, with a largest value in size bin 2 (156–625 nm). The values in the eastern coastal and relatively clean areas were generally larger than those in inland and polluted areas due to variations of relative humidity (RH), and were suppressed in nitrate dominated areas. Scheme Riemer09 is related to the thickness of SOA (secondary organic aerosol) package (l/Rp) and produced at least 2 μg/m³ of nitrate inhibition in regions where l/Rp ≥ 0.08 fit

γ_{D}

(the uptake coefficient of inorganic core) ≥ 1 × 10⁻². Scheme Gaston14 considers the effects of ambient RH and SOA phase; in those areas where RH was greater than 70 %, the coating effect simulated by scheme Gaston14 was relatively small; when low RH (<40 %) and low O:C ratios (<0.48) coexisted, scheme Gaston14 had a significant coating effect, leading to its simulated nitrate being ∼4 μg/m³ lower than the simulation of scheme Riemer09. The two coating schemes showed a similar vertical trend, with a maximum difference of 15 % of the heterogeneous produced nitrate in size bin 2 in the polluted areas at the height of ∼240m. Scheme Gaston14 exhibited greater advantages under complex meteorological and aerosol conditions.

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来源期刊

Atmospheric Environment 环境科学-环境科学

CiteScore

9.40

自引率

8.00%

发文量

458

审稿时长

53 days

期刊介绍： Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.