Zeng Jianhui, Xu Wanyun, Kuang Ye, Xu Weiqi, Liu Chang, Zhang Gen, Zhao Huarong, Ren Sanxue, Zhou Guangsheng, Xu Xiaobin
State Key Laboratory of Severe Weather, Key Laboratory for Atmospheric Chemistry, Institute of Atmospheric Composition, Chinese Academy of Meteorological Sciences, Beijing 100081, China.
Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, China.
Toxics. 2024 Apr 30;12(5):331. doi: 10.3390/toxics12050331.
Solar radiation triggers atmospheric nitrous acid (HONO) photolysis, producing OH radicals, thereby accelerating photochemical reactions, leading to severe secondary pollution formation. Missing daytime sources were detected in the extensive HONO budget studies carried out in the past. In the rural North China Plain, some studies attributed those to soil emissions and more recent studies to dew evaporation. To investigate the contributions of these two processes to HONO temporal variations and unknown production rates in rural areas, HONO and related field observations obtained at the Gucheng Agricultural and Ecological Meteorological Station during spring and autumn were thoroughly analyzed. Morning peaks in HONO frequently occurred simultaneously with those of ammonia (NH) and water vapor both during spring and autumn, which were mostly caused by dew and guttation water evaporation. In spring, the unknown HONO production rate revealed pronounced afternoon peaks exceeding those in the morning. In autumn, however, the afternoon peak was barely detectable compared to the morning peak. The unknown afternoon HONO production rates were attributed to soil emissions due to their good relationship to soil temperatures, while NH soil emissions were not as distinctive as dew emissions. Overall, the relative daytime contribution of dew emissions was higher during autumn, while soil emissions dominated during spring. Nevertheless, dew emission remained the most dominant contributor to morning time HONO emissions in both seasons, thus being responsible for the initiation of daytime OH radical formation and activation of photochemical reactions, while soil emissions further maintained HONO and associated OH radial formation rates at a high level, especially during spring. Future studies need to thoroughly investigate the influencing factors of dew and soil emissions and establish their relationship to HONO emission rates, form reasonable parameterizations for regional and global models, and improve current underestimations in modeled atmospheric oxidation capacity.
太阳辐射引发大气中的亚硝酸(HONO)光解,产生羟基自由基,从而加速光化学反应,导致严重的二次污染形成。在过去开展的广泛的HONO收支研究中检测到了白天来源缺失的情况。在中国北方农村平原地区,一些研究将其归因于土壤排放,而最近的研究则归因于露水蒸发。为了研究这两个过程对农村地区HONO时间变化和未知产生率的贡献,对春季和秋季在古城农业与生态气象站获得的HONO及相关实地观测数据进行了全面分析。在春季和秋季,HONO的早晨峰值经常与氨(NH₃)和水汽的早晨峰值同时出现,这主要是由露水和吐水蒸发引起的。在春季,未知的HONO产生率在下午出现明显峰值,超过早晨峰值。然而,在秋季,与早晨峰值相比,下午峰值几乎检测不到。未知下午HONO产生率归因于土壤排放,因为它们与土壤温度有良好的关系,而NH₃土壤排放不如露水排放那么明显。总体而言,秋季露水排放的白天相对贡献较高,而春季土壤排放占主导。尽管如此,露水排放在两个季节中仍然是早晨时段HONO排放的最主要贡献者,因此是白天羟基自由基形成起始和光化学反应活化的原因,而土壤排放进一步将HONO及相关羟基自由基形成速率维持在较高水平,特别是在春季。未来的研究需要深入调查露水和土壤排放的影响因素,建立它们与HONO排放率的关系,为区域和全球模型形成合理的参数化,并改善当前模型中对大气氧化能力的低估。