Rising frequency of ozone-favorable synoptic weather patterns contributes to 2015-2022 ozone increase in Guangzhou.

Objective weather classification methods have been extensively applied to identify dominant ozone-favorable synoptic weather patterns (SWPs), however, the consistency of different classification methods is rarely examined. In this study, we apply two widely-used objective methods, the self-organizing map (SOM) and K-means clustering analysis, to derive ozone-favorable SWPs at four Chinese megacities in 2015-2022. We find that the two algorithms are largely consistent in recognizing dominant ozone-favorable SWPs for four Chinese megacities. In the case of classifying six SWPs, the derived circulation fields are highly similar with a spatial correlation of 0.99 between the two methods, and the difference in the mean frequency of each SWP is less than 7%. The six dominant ozone-favorable SWPs in Guangzhou are all characterized by anomaly higher radiation and temperature, lower cloud cover, relative humidity, and wind speed, and stronger subsidence compared to climatology mean. We find that during 2015-2022, the occurrence of ozone-favorable SWPs days increases significantly at a rate of 3.2 day/year, faster than the increases in the ozone exceedance days (3.0 day/year). The interannual variability between the occurrence of ozone-favorable SWPs and ozone exceedance days are generally consistent with a temporal correlation coefficient of 0.6. In particular, the significant increase in ozone-favorable SWPs in 2022, especially the Subtropical High type which typically occurs in September, is consistent with a long-lasting ozone pollution episode in Guangzhou during September 2022. Our results thus reveal that enhanced frequency of ozone-favorable SWPs plays an important role in the observed 2015-2022 ozone increase in Guangzhou.

Tower-based profiles of wintertime secondary organic aerosols in the urban boundary layer over Guangzhou.

Secondary organic aerosol (SOA) accounts for a large fraction of fine particulate matter (PM2.5), but the lack of vertical observations of SOA in the urban boundary layer (UBL) limits a comprehensive understanding of its sources and formation mechanisms. In this study, PM2.5 samples were simultaneously collected at 3 m, 118 m, and 488 m on the Canton Tower in Guangzhou during winter. Typical SOA tracers, including oxidation products of isoprene (SOAI), monoterpene (SOAM), sesquiterpene (SOAS), and toluene (ASOA), were investigated alongside meteorological parameters and gaseous/particulate pollutants. Total concentrations of SOA tracers showed an increasing trend with height, with daytime levels exceeding nighttime levels. C5-alkene triols and 2-methylglyceric acid displayed a significant increase with height, potentially affected by nighttime chemistry in the residual layer, determining the overall vertical trend of SOAI tracers. Concentrations of later-generation SOAM (SOAM_S) tracers also increased with height, while those of first-generation SOAM (SOAM_F) tracers decreased, indicating relatively aged SOAM in the upper layers. SOAS and ASOA tracers exhibited higher enhancement under polluted conditions, likely impacted by biomass burning and anthropogenic emissions. The yields of SOAI tracers varied with temperature in the vertical profile. The formation of SOAM_F tracers was negatively correlated with relative humidity, liquid water content, and pH, affecting their vertical distributions. The effect of O3 on SOA formation enhanced significantly with height, influenced by air mass transport, and likely contributed to the higher yields of SOA in the upper layer. However, at ground level, SOA formation was primarily driven by high local emissions of both NOx and volatile organic compounds. We also observed the roles of SO2 in SOA generation, particularly at 118 m. This study demonstrates the vertical diurnal characteristics of SOA tracers in the UBL, highlighting the varying effects of meteorological conditions and anthropogenic pollutants on SOA formation at different heights.

Influence of boundary layer jets on the vertical distribution of ozone in Guangdong, China.

The planetary boundary layer (PBL) characteristics during ozone (O3) episodes in China have been extensively studied; however, knowledge of the impact of boundary layer jets (BLJs) on O3 vertical distribution is limited. This study conducted a field campaign from 1 to 8 December 2020 to examine the vertical structure of the O3 concentration and wind velocity within the boundary layer at two sites (Foshan: FS, Maoming: MM) in Guangdong. Utilising lidar observations and the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), distinct spatial distribution patterns of O3 over FS and MM influenced by BLJs were identified. The BLJs at both locations exhibited pronounced diurnal variations with a nocturnal maximum exceeding 11 m/s at a height of approximately 500 m. The nocturnal enhancement of BLJs resulted from inertial oscillations coupled with diurnal thermal forcing over sloping terrain. A stronger BLJ at FS induced an evident uplift of O3 and the prevailing northeasterly wind facilitated the transport of O3 in the nocturnal residual layer from FS to MM. After sunrise, surface heating and the development of the PBL caused the air mass with elevated O3 levels in the residual layer to descend to ground level. At MM, calm surface winds, a weaker BLJ at 500 m height, and strong downdrafts collectively contributed to a significant increase in surface O3 concentration in subsequent days. These findings contribute to our understanding of the interactions between BLJs and variations in surface air pollutant concentrations, thereby providing important insights for future regional emissions control measures.

Soil Emissions of Reactive Nitrogen Accelerate Summertime Surface Ozone Increases in the North China Plain.

Summertime surface ozone in China has been increasing since 2013 despite the policy-driven reduction in fuel combustion emissions of nitrogen oxides (NOx). Here we examine the role of soil reactive nitrogen (Nr, including NOx and nitrous acid (HONO)) emissions in the 2013-2019 ozone increase over the North China Plain (NCP), using GEOS-Chem chemical transport model simulations. We update soil NOx emissions and add soil HONO emissions in GEOS-Chem based on observation-constrained parametrization schemes. The model estimates significant daily maximum 8 h average (MDA8) ozone enhancement from soil Nr emissions of 8.0 ppbv over the NCP and 5.5 ppbv over China in June-July 2019. We identify a strong competing effect between combustion and soil Nr sources on ozone production in the NCP region. We find that soil Nr emissions accelerate the 2013-2019 June-July ozone increase over the NCP by 3.0 ppbv. The increase in soil Nr ozone contribution, however, is not primarily driven by weather-induced increases in soil Nr emissions, but by the concurrent decreases in fuel combustion NOx emissions, which enhance ozone production efficiency from soil by pushing ozone production toward a more NOx-sensitive regime. Our results reveal an important indirect effect from fuel combustion NOx emission reduction on ozone trends by increasing ozone production from soil Nr emissions, highlighting the necessity to consider the interaction between anthropogenic and biogenic sources in ozone mitigation in the North China Plain.

Observation-derived 2010-2019 trends in methane emissions and intensities from US oil and gas fields tied to activity metrics.

The United States is the world's largest oil/gas methane emitter according to current national reports. Reducing these emissions is a top priority in the US government's climate action plan. Here, we use a 2010 to 2019 high-resolution inversion of surface and satellite observations of atmospheric methane to quantify emission trends for individual oil/gas production regions in North America and relate them to production and infrastructure. We estimate a mean US oil/gas methane emission of 14.8 (12.4 to 16.5) Tg a-1 for 2010 to 2019, 70% higher than reported by the US Environmental Protection Agency. While emissions in Canada and Mexico decreased over the period, US emissions increased from 2010 to 2014, decreased until 2017, and rose again afterward. Increases were driven by the largest production regions (Permian, Anadarko, Marcellus), while emissions in the smaller production regions generally decreased. Much of the year-to-year emission variability can be explained by oil/gas production rates, active well counts, and new wells drilled, with the 2014 to 2017 decrease driven by reduction in new wells and the 2017 to 2019 surge driven by upswing of production. We find a steady decrease in the oil/gas methane intensity (emission per unit methane gas production) for almost all major US production regions. The mean US methane intensity decreased from 3.7% in 2010 to 2.5% in 2019. If the methane intensity for the oil/gas supply chain continues to decrease at this pace, we may expect a 32% decrease in US oil/gas emissions by 2030 despite projected increases in production.

Quantitative evaluation of impacts of the steadiness and duration of urban surface wind patterns on air quality.

The complexity and heterogeneity of urban land surfaces result in inconsistencies in near-surface winds, which in turn influence the diffusion and dispersion of air pollutants. In this study, we classified urban surface wind fields, quantified their steadiness, duration, and influence on air quality using hourly wind observations from 50 meteorological stations, as well as hourly PM2.5 and NO2 concentrations from 18 monitoring stations during 2017-2018 in Shenzhen, a mega city in southern China. We found that the K-means clustering technique was reliable for distinguishing surface wind patterns within the city. Urban surface-wind patterns greatly affected pollutant concentrations. When dominated by calm, northerly wind, high PM2.5/NO2 concentration episodes occurred more frequently than those during other surface wind patterns. The urban surface transport index (USTI) was used to quantify the steadiness of surface wind classes. High pollutant concentrations were present during both high wind speed periods with a large USTI, indicating external pollutant transport, and during low wind speed periods with a small USTI, indicating pollutant accumulation. The threshold durations for surface wind fields (TDSWF) was proposed to quantify the impacts of surface wind persistence on air quality. We found that poor air quality occurred during the first several hours of a dominant wind pattern, indicating that transitions between wind patterns should be a particular focus when assessing air-quality deterioration. USTI and TDSWF are potentially applicable to other urban areas, owing to their clear definitions and simple calculation. In combination with wind speeds, these indices are likely to improve air quality forecasting and strategic decisions on air pollution emergencies, based on long time series of multiple wind and pollutant concentration observations.

[Effects of Tropical Cyclones on Ozone Pollution in the Pearl River Delta in Autumn].

Based on the tropical cyclone track data in the northwest Pacific Ocean from 2015 to 2020, meteorological observation data, and ozone concentration monitoring data in the Pearl River Delta (PRD), the impacts of four tropical cyclones, namely the westbound tropical cyclone (type A), East China Sea tropical cyclone (type B), offshore tropical cyclone (type C), and offshore tropical cyclone (type D), on ozone concentration in the PRD were analyzed. The results showed that:under the influence of the type A tropical cyclone, the risk of regional ozone concentration exceeding the standard exhibited little change. Under the influence of the type B tropical cyclone, the risk of ozone exceeding the standard in the PRD was obviously increased. Under the influence of the type C tropical cyclone, the risk of regional ozone exceeding the standard obviously increased, but the increase was weaker than that of the type B tropical cyclone. The type D tropical cyclone was far away from the Chinese mainland and had little influence on ozone concentration in the PRD. When the type A or type C tropical cyclones occurred, the average daily maximum 8-hour average ozone concentration (MDA8) in the PRD region increased by approximately 5 µg·m-3, and the ozone MDA8 in some cities may have decreased. When the type B tropical cyclone occurred, the regional ozone MDA8 increased by 19 µg·m-3 on average, and the ozone concentration in all cities increased significantly. Among them, the average increase in ozone MDA8 in Zhuhai and Jiangmen was relatively large, with an increase of greater than 20 µg·m-3. Generally speaking, the ozone concentration in cities in the western PRD was more affected by tropical cyclones. When the type B tropical cyclone occurred, solar radiation increased, sunshine duration lengthened, cloud cover decreased, air temperature rose, and relative humidity decreased in the PRD, all of which were beneficial to photochemical reactions. Meanwhile, downward flow increased in the boundary layer, and downward flow transported high-concentration ozone to the ground, which promoted the increase in ozone concentration on the ground. When type A or type C tropical cyclones occurred, the change in meteorological conditions was not entirely conducive to the increase in ozone concentration, and in some cases, even adverse meteorological conditions such as rainfall occurred, which led to the risk of regional ozone exceeding the standard being less than that of the type B tropical cyclone. Affected by tropical cyclones, sunshine hours and air temperature in western cities of the PRD increased more than those in eastern cities, which was more conducive to ozone generation.

A cold front induced co-occurrence of O3 and PM2.5 pollution in a Pearl River Delta city: Temporal variation, vertical structure, and mechanism.

In this study, the spatiotemporal variabilities and characteristics of ozone (O3) and fine particulate matter (PM2.5) were reconstructed, and the interaction between meteorological conditions and the co-occurrence of O3 and PM2.5 in Zhuhai, a city in the Pearl River Delta (China), was analysed. The vertical distributions of lower tropospheric O3, aerosol extinction coefficient, and wind velocity were measured using a ground-based LiDAR system. The diurnal variations in air pollutant concentrations and meteorological conditions at ground level were examined from 28 November to December 8, 2020 considering the weather conditions in Zhuhai. Heavy pollution episodes with increased concentrations of O3 and PM2.5 were observed from 6 to 7 December after a period of cold air invasion. The maximum hourly average concentrations of O3 and PM2.5 at the ground level reached up to 190 µg/m3, 98 µg/m3, respectively. The horizontal wind speed rapidly decreased to less than 2 m/s during the heavy pollution episodes driven by O3 and PM2.5, whereas the vertical wind velocity was dominated by the downdraught. When the large-scale synoptic winds were weak, a strengthening sea breeze in the afternoon could promote the landward propagation of warm marine air masses, and a lower surface wind speed was driven by the convergence of cold air from the north and warm air from the south. In turn, this increased the residence time of air pollutants and promoted their conversion to secondary pollutants. Regarding the pollution sources, the results indicated that the Pearl River Estuary represented a 'pool' of O3 and PM2.5 pollution. In addition, the contribution of regional pollutant transport could not be ignored when considering the accumulative increase in air pollution. Overall, the relatively weak synoptic winds, low mixing height, and high generation of pollution around Zhuhai collectively resulted in high concentrations of O3 and PM2.5.

Response surface model based emission source contribution and meteorological pattern analysis in ozone polluted days.

Urban and regional ozone (O3) pollution is a public health concern and causes damage to ecosystems. Due to the diverse emission sources of O3 precursors and the complex interactions of air dispersion and chemistry, identifying the contributing sources of O3 pollution requires integrated analysis to guide emission reduction plans. In this study, the meteorological characteristics leading to O3 polluted days (in which the maximum daily 8-h average O3 concentration is higher than the China Class II National O3 Standard (160 µg/m3)) in Guangzhou (GZ, China) were analyzed based on data from 2019. The O3 formation regimes and source apportionments under various prevailing wind directions were evaluated using a Response Surface Modeling (RSM) approach. The results showed that O3 polluted days in 2019 could be classified into four types of synoptic patterns (i.e., cyclone, anticyclone, trough, and high pressure approaching to sea) and were strongly correlated with high ambient temperature, low relative humidity, low wind speed, variable prevailing wind directions. Additionally, the cyclone pattern strongly promoted O3 formation due to its peripheral subsidence. The O3 formation was nitrogen oxides (NOx)-limited under the northerly wind, while volatile organic compounds (VOC)-limited under other prevailing wind directions. Anthropogenic emissions contributed largely to the O3 formation (54-78%) under the westerly, southwesterly, easterly, southeasterly, or southerly wind, but only moderately (35-47%) under the northerly or northeasterly wind. Furthermore, as for anthropogenic contributions, local emission contributions were the largest (39-60%) regardless of prevailing wind directions, especially the local NOx contributions (19-43%); the dominant upwind regional emissions contributed 12-46% (e.g., contributions from Dongguan were 12-20% under the southeasterly wind). The emission control strategies for O3 polluted days should focus on local emission sources in conjunction with the emission reduction of upwind regional sources.