Assessment of the H2O2 budget at an urban site concerning the HO2 underprediction and the vertical transport from residual layers
Assessment of the H2O2 budget at an urban site concerning the HO2 underprediction and the vertical transport from residual layers
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评估城市场地的 H2O2 预算，涉及 HO2 预测不足和残余层的垂直传输
DOI：
10.1016/j.atmosenv.2022.118952
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发表时间：
2022-01
影响因子：
5
通讯作者：
Zhang Xiaoshan
中科院分区：
文献类型：
--
作者：
Guo Jia;Wang Zhe;Cui Yaru;Zhang Xiaoshan
于2018年9月23日至11月4日在北京市某城区进行了H2 O2现场观测。在测量期间，H2 O2和有机过氧化物（OP）的日峰值浓度分别为0.57 ppbv（范围：0.07-1.89 ppbv）和0.16 ppbv（范围：0.06-0.35 ppbv）。使用基于观测的模式，模拟的HO 2水平再现了一个低得多的H2 O2生产率比观测，特别是在上午弱风，非湍流地面风条件下。在此基础上，对模拟的H2 O2浓度进行修正后，H2 O2的日累积产生率增加了144%~ 164%，这对解释轻度污染和污染日的高H2 O2具有重要意义，但仍不足以解释。H2 O2对气溶胶的异质性生产和H2 O2去除率的高估进行了检查，而不是这个额外的H2 O2缺失源的根本原因。H2 O2残留层的浓度进行了评价。残积层对H2 O2的储集作用强于对O3的储集作用。在非湍流条件下的城市站点，上午的残留层H2 O2估计约为地面H2 O2在空气层垂直混合之前的20-80倍。垂直混合对上午地面H2 O2浓度有显著影响。这项工作强调了在大气H2 O2研究中考虑HO 2低估和空气质量垂直混合的重要性。
Field observation of H2O2was conducted at an urban site in Beijing from Sep.23rd to Nov.4th of 2018. The daily peak concentrations of H2O2and organic peroxides (OPs) during the measurement were 0.57 ppbv (Range: 0.07–1.89 ppbv) and 0.16 ppbv (Range 0.06–0.35 ppbv). Using an observation based model, the modeled HO2level reproduced a much lower H2O2production rate than the observation, especially in the morning under the weak wind, non-turbulent surface winds conditions. With the modeled-HO2concentration corrected based on the previously reported observed/modeled HO2ratio in this city, the daily integrated H2O2production rate increased by 144%–164%, which is important but still not enough to explain the observed high H2O2in the lightly polluted and polluted days. Heterogeneous production of H2O2on aerosols and the overestimation of H2O2removal rates were examined not the underlying causes of this additional H2O2missing source. H2O2concentrations in residual layers were evaluated. The residual layer was revealed a stronger reservoir of H2O2than its reservoir effect on O3. In the morning of non-turbulent conditions at the urban site, the residual layers H2O2were estimated about 20–80 times of the ground surface H2O2before the air layers vertical mixing. The vertical mixing significantly affects gaseous H2O2concentration on the ground in the morning. This work highlights the importance to consider the HO2underestimation and air mass vertical mixing in atmospheric H2O2studies.
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