Wang Runyu, Wang Lili, Sun Jiaren, Zhang Lei, Li Yuanyuan, Li Ke, Liu Boya, Zhang Jiaxin, Wang Yuesi
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China; College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China.
Sci Total Environ. 2023 Dec 20;905:166987. doi: 10.1016/j.scitotenv.2023.166987. Epub 2023 Sep 17.
The Pearl River Delta (PRD) has long been plagued by severe O pollution, particularly during the autumn. A regional O pollution episode influenced by the Western Pacific Subtropical High in September 2021 was characterized by near-surface O escalation due to strong photochemical reactions within the planetary boundary layer. This event was targeted to develop effective control strategies through investigation of precursor control type and scope based on the high-order decoupled direct method (HDDM) and integrated source apportionment method (ISAM) of CMAQ. Generally, the majority of areas (67.0 %) were under NO-limited regime, which should strengthen afternoon NO control inferred by positive convex O responses. However, high emission and heavily polluted areas located in central PRD were under VOC-limited regime (11.6 %) or mixed regime (15.0 %). The remaining areas (6.4 %) were under NO-titration or insensitive conditions. Regarding source apportionment, Guangdong province contributed 32.3 %-58.4 % to MDA8 O of PRD, especially higher proportion (>50 %) to central areas. Overall, local-focused NO/VOC emission reductions had limited effects on O mitigation for receptor cities compared to regional-cooperative regulation. When region-wide VOC emission reduction was implemented, MDA8 O in VOC-limited grids exhibited the largest declines (2.3 %-4.1 %, 3.9- 7.0 μg·m). However, unified NO control contributed to increasing MDA8 O in VOC-limited grids (most stations located for air quality evaluation) whereas decreased MDA8 O by 2.1 %- 5.7 %, 3.0- 8.2 μg·m in large-scale NO-limited grids. The sensitivity-oriented regional control avoided O rebound and achieved the greatest decline of 3.4 %- 5.0 %, 5.7- 8.4 μg·m in VOC-limited grids; additionally, time-refined dynamic aggressive NO control decreased peak O by an extra 1.2- 6 μg·m, both of which facilitate the regulation for the forecasting O episodes. These findings suggest that in heavily polluted environments, the enhancement of O regulation benefits requires meticulous, coordinated, and dynamic NO and VOC controls spanning the entire region based on high-resolution analysis of heterogeneous O-NO-VOC sensitivity. Furthermore, emission reduction gains should be more reasonably reflected through increasing in-situ observations covering multi-sensitivity regions.
长期以来,珠江三角洲一直饱受严重的臭氧污染困扰,尤其是在秋季。2021年9月受西太平洋副热带高压影响的一次区域臭氧污染事件,其特征是由于行星边界层内强烈的光化学反应导致近地面臭氧浓度升高。该事件旨在通过基于CMAQ的高阶解耦直接法(HDDM)和综合源解析方法(ISAM)调查前体物控制类型和范围,来制定有效的控制策略。总体而言,大部分地区(67.0%)处于氮氧化物限制状态,根据臭氧的正凸响应推断,应加强下午时段对氮氧化物的控制。然而,位于珠江三角洲中部的高排放和重污染地区处于挥发性有机物限制状态(11.6%)或混合状态(15.0%)。其余地区(6.4%)处于氮氧化物滴定或不敏感状态。关于源解析,广东省对珠江三角洲日最大8小时平均臭氧的贡献率为32.3% - 58.4%,对中部地区的贡献率尤其更高(>50%)。总体而言,与区域协同监管相比,以本地为重点的氮氧化物/挥发性有机物减排对受体城市的臭氧减排效果有限。当实施全区域挥发性有机物减排时,挥发性有机物限制网格中的日最大8小时平均臭氧下降幅度最大(2.3% - 4.1%,3.9 - 7.0微克·立方米)。然而,统一控制氮氧化物导致挥发性有机物限制网格(大多数站点用于空气质量评估)中的日最大8小时平均臭氧增加,而在大规模氮氧化物限制网格中日最大8小时平均臭氧下降了2.1% - 5.7%,3.0 - 8.2微克·立方米。以敏感性为导向的区域控制避免了臭氧反弹,并在挥发性有机物限制网格中实现了最大降幅3.4% - 5.0%,5.7 - 8.4微克·立方米;此外,时间精细化动态积极氮氧化物控制使臭氧峰值额外降低了1.2 - 6微克·立方米,这两者都有助于对臭氧污染事件进行预测的监管。这些研究结果表明,在重污染环境中,要提高臭氧监管效益,需要基于对臭氧 - 氮氧化物 - 挥发性有机物非均匀敏感性的高分辨率分析,在整个区域进行细致、协调和动态的氮氧化物和挥发性有机物控制。此外,减排成效应通过增加覆盖多敏感性区域的现场观测更合理地体现出来。