利用 TROPOMI HCHO 观测数据约束非甲烷挥发性有机化合物排放:对 2022 年 8 月中国夏季臭氧模拟的影响

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Atmospheric Chemistry and Physics Pub Date : 2024-07-02 DOI:10.5194/acp-24-7481-2024
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, Weimin Ju
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引用次数: 0

摘要

摘要非甲烷挥发性有机化合物(NMVOC)是 O3 的重要前体,对大气氧化能力和 O3 的形成有重大影响。然而,人为和生物产生的非甲烷挥发性有机化合物排放仍然存在很大的不确定性。在此,我们使用集合卡尔曼滤波(EnKF)算法扩展了区域多空气污染物同化系统(RAPAS),通过同化 TROPOspheric Monitoring Instrument (TROPOMI) HCHO 检索数据,优化了 2022 年 8 月中国的 NMVOC 排放。我们还同时通过同化现场二氧化氮观测数据来优化氮氧化物的排放,以解决挥发性有机物-氮氧化物-臭氧之间的化学反馈问题。此外,我们还采用了基于过程的分析方法,以量化 NMVOC 排放变化对与 O3 形成和耗竭相关的各种化学反应的影响。NMVOC 排放量大幅减少了 50.2%,尤其是在长江中下游地区,这揭示了之前由于极端热浪而高估的生物源 NMVOC 排放量。与先期 NMVOC 排放预测相比,后期排放预测显著改善了 HCHO 模拟,偏差减少了 75.7%,表明后期排放的不确定性明显降低。后排放预测还有效纠正了先排放预测中对臭氧的高估,将偏差减少了 49.3%。这主要归因于下午的 RO2+NO 反应速率显著下降,NO2+OH 反应速率上升,从而限制了 O3 的生成。敏感性分析强调,要全面评估 O3 化学性质,必须同时考虑 NMVOC 和 NOx 的排放。这项研究加深了我们对 NMVOC 排放对 O3 生成的影响的理解,有助于制定有效的减排政策。
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Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Abstract. Non-methane volatile organic compounds (NMVOC), serving as crucial precursors of O3, have a significant impact on atmospheric oxidative capacity and O3 formation. However, both anthropogenic and biogenic NMVOC emissions remain subject to considerable uncertainty. Here, we extended the Regional multi-Air Pollutant Assimilation System (RAPAS) using the ensemble Kalman filter (EnKF) algorithm to optimize NMVOC emissions in China in August 2022 by assimilating TROPOspheric Monitoring Instrument (TROPOMI) HCHO retrievals. We also simultaneously optimize NOx emissions by assimilating in situ NO2 observations to address the chemical feedback among VOCs–NOx–O3. Furthermore, a process-based analysis was employed to quantify the impact of NMVOC emission changes on various chemical reactions related to O3 formation and depletion. NMVOC emissions exhibited a substantial reduction of 50.2 %, especially in the middle and lower reaches of the Yangtze River, revealing a prior overestimation of biogenic NMVOC emissions due to an extreme heat wave. Compared to the forecast with prior NMVOC emissions, the forecast with posterior emissions significantly improved HCHO simulations, reducing biases by 75.7 %, indicating a notable decrease in posterior emission uncertainties. The forecast with posterior emissions also effectively corrected the overestimation of O3 in forecasts with prior emissions, reducing biases by 49.3 %. This can be primarily attributed to a significant decrease in the RO2+NO reaction rate and an increase in the NO2+OH reaction rate in the afternoon, thus limiting O3 generation. Sensitivity analyses emphasized the necessity of considering both NMVOC and NOx emissions for a comprehensive assessment of O3 chemistry. This study enhances our understanding of the effects of NMVOC emissions on O3 production and can contribute to the development of effective emission reduction policies.
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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