Modeling the molecular composition of secondary organic aerosol under highly polluted conditions: A case study in the Yangtze River Delta Region in China.

A near-explicit mechanism, the master chemical mechanism (MCMv3.3.1), coupled with the Community Multiscale Air Quality (CMAQ) model (CMAQ-MCM-SOA), was applied to investigate the characteristics of secondary organic aerosol (SOA) during a pollution event in the Yangtze River Delta (YRD) region in summer 2018. Model performances in predicting explicit volatile organic compounds (VOCs), organic aerosol (OA), secondary organic carbon (SOC), and other related pollutants in Taizhou, as well as ozone (O3) and fine particulate matter (PM2.5) in multiple cities in this region, were evaluated against observations and model predictions by the CMAQ model coupled with a lumped photochemical mechanism (SAPRC07tic, S07). MCM and S07 exhibited similar performances in predicting gaseous species, while MCM better captured the observed PM2.5 and inorganic aerosols. Both models underpredicted OA concentrations. When excluding data during biomass burning events, SOC concentrations were underpredicted by the CMAQ-MCM-SOA model (-28.4 %) and overpredicted by the CMAQ-S07 model (134.4 %), with better agreement with observations in the trend captured by the CMAQ-MCM-SOA model. Dicarbonyl SOA accounted for a significant fraction of total SOA in the YRD, while organic nitrates originating from aromatics were the most abundant species contributing to the SOA formation from gas-particle partitioning. The oxygen-to­carbon ratio (O/C) for SOA and OA were 0.68-0.75 and 0.20-0.65, respectively, indicating a higher oxidation state in the areas influenced by biogenic emissions. Finally, the phase state of SOA was examined by calculating the glass transition temperature (Tg) based on its molecular composition. It was found that semi-solid state characterized SOA in the YRD, which could potentially impact their chemical transformation and lifetimes along with those of their precursors.

[Differences of Three Methods in Determining Ozone Sensitivity in Nanjing].

In recent years， ozone （O3） has become an increasingly important air pollutant in China. Identifying the sensitivity of O3 to the precursors volatile organic compounds （VOCs） and nitrogen oxides （NOx） can help make effective abatement strategies. This study compared three methods for determining O3-VOCs-NOx sensitivity： simulated photochemical indicator values and sensitivity coefficients derived from a three-dimensional air quality model and an observation-based model （OBM）， with a case study involving an O3 pollution event that occurred in Nanjing in late July 2017. The results showed that O3 sensitivity based on the photochemical indicator and sensitivity coefficients demonstrated similar spatial variations （over 50% of the grid cells of Nanjing exhibiting identical O3 sensitivity）. However， sensitivity coefficients identified a larger number of areas within a transitional O3 sensitivity regime， as opposed to the VOCs- or NOx-limited regime identified by the photochemical indicator. The determination of the latter was affected by the adopted threshold values. The OBM relied on the quality of the observational data. For example， positive biases in observed NO2 could lead to an underestimation of O3 sensitivity to NOx with the OBM. During the high pollution period， the three methods exhibited significant disparities. The photochemical indicator tended to suggest the VOCs-limited condition， whereas the OBM and sensitivity coefficients indicated the NOx-limited or transitional regimes.

[Impacts of Anthropogenic Emission Reduction on Urban Atmospheric Oxidizing Capacity During the COVID-19 Lockdown].

In recent years， regional compound air pollution events caused by fine particles （PM2.5） and ozone （O3） have occurred frequently in economically developed areas of China， in which atmospheric oxidizing capacity （AOC） has played an important role. In this study， the WRF-CMAQ model was used to study the impacts of anthropogenic emission reduction on AOC during the COVID-19 lockdown period. Three representative cities in eastern China （Shijiazhuang， Nanjing， and Guangzhou） were selected for an in-depth analysis to quantify the contribution of meteorology and emissions to the changes in AOC and oxidants and to discuss the impact of AOC changes on the formation of secondary pollutants. The results showed that， compared with that in the same period in 2019， the urban average AOC in Shijiazhuang， Nanjing， and Guangzhou in 2020 increased by 60%， 48.7%， and 12.6%， respectively. The concentrations of O3， hydroxyl radical （·OH）， and nitrogen trioxide （NO3·ï¼‰ increased by 1.6%-26.4%， 14.8%-73.3%， and 37.9%-180%， respectively. The AOC in the three cities increased by 0.06×10-4， 0.12×10-4， and 0.33×10-4 min-1， respectively， due to emission reduction. The meteorological change increased AOC in Shijiazhuang and Nanjing by 20% and 17.9%， respectively， but decreased AOC in Guangzhou by -9.3%. Enhanced AOC led to an increase in the nitrogen oxidation ratio （NOR） and VOCs oxidation ratio （VOR） and promoted the transformation of primary pollutants to secondary pollutants. This offset the effects of primary emission reduction and resulted in a nonlinear decline in secondary pollutants compared to emissions during the COVID-19 lockdown.

[Elucidating the Impacts of Meteorology and Emission Changes on Concentrations of Major Air Pollutants in Major Cities in the Yangtze River Delta Region Using a Machine Learning De-weather Method].

This study applied a de-weather method based on a machine learning technique to quantify the contribution of meteorology and emission changes to air quality from 2015 to 2021 in four cities in the Yangtze River Delta Region. The results showed that the significant reductions in PM2.5, NO2, and SO2 emissions(57.2%-68.2%, 80.7%-94.6%, and 81.6%-96.1%, respectively) offset the adverse effects of meteorological conditions, resulting in lower pollutant concentrations. The meteorological contribution of maximum daily 8-h average O3(MDA8_O3) showed a stronger effect than that of others(23.5%-42.1%), and meteorological factors promoted the increase in MDA8_O3 concentrations(4.7%); however, emission changes overall resulted in a decrease in MDA8_O3 concentrations(-3.2%). NO2 and MDA8_O3 decreased more rapidly from 2019 to 2021, mainly because the emissions played a stronger role in reducing pollutant concentrations than from 2015 to 2018. However, emissions changes had weaker reduction effects on PM2.5 and SO2 from 2019 to 2021 than from 2015 to 2018. De-weather methods could effectively seperate the effects of meteorology and emission changes on pollutant trends, which helps to evaluate the real effects of emission control policies on pollutant concentrations.

Fate of Oxygenated Volatile Organic Compounds in the Yangtze River Delta Region: Source Contributions and Impacts on the Atmospheric Oxidation Capacity.

The Community Multiscale Air Quality model (CMAQv5.2) was implemented to investigate the sources and sinks of oxygenated volatile organic compounds (OVOCs) during a high O3 and high PM2.5 season in the Yangtze River Delta (YRD) region, based on constraints from observations. The model tends to overpredict non-oxygenated VOCs and underpredict OVOCs, which has been improved with adjusted emissions of all VOCs. The OVOCs in the YRD are dominated by ketones, aldehydes, and alcohols. Ketones and aldehydes mainly originate from direct emissions and secondary formation in the northern YRD, and primarily originate from secondary formation in the southern part influenced by biogenic emissions. The concentration of secondary organic aerosols (SOA) produced by OVOCs is 0.5-1.5 µg/m3, with 40-80% originated from organic nitrates, 20-70% originated from dicarbonyls, and 0-20% originated from isoprene epoxydiols. The influences of OVOCs on the atmospheric oxidation capacity are dominated by the OH• pathway during the day (∼350%) and by the NO3• pathway at night (∼150%). Consequently, O3 is enhanced by 30-70% in the YRD. Aerosols are also enhanced by 50-140%, 20-80%, and ∼20% for SOA, nitrate, and sulfate, respectively.

Modeling particulate nitrate in China: Current findings and future directions.

Particulate nitrate (pNO3) is now becoming the principal component of PM2.5 during severe winter haze episodes in many cities of China. To gain a comprehensive understanding of the key factors controlling pNO3 formation and driving its trends, we reviewed the recent pNO3 modeling studies which mainly focused on the formation mechanism and recent trends of pNO3 as well as its responses to emission controls in China. The results indicate that although recent chemical transport models (CTMs) can reasonably capture the spatial-temporal variations of pNO3, model-observation biases still exist due to large uncertainties in the parameterization of dinitrogen pentoxide (N2O5) uptake and ammonia (NH3) emissions, insufficient heterogeneous reaction mechanism, and the predicted low sulfate concentrations in current CTMs. The heterogeneous hydrolysis of N2O5 dominates nocturnal pNO3 formation, however, the contribution to total pNO3 varies among studies, ranging from 21.0% to 51.6%. Moreover, the continuously increasing PM2.5 pNO3 fraction in recent years is mainly due to the decreased sulfur dioxide emissions, the enhanced atmospheric oxidation capacity (AOC), and the weakened nitrate deposition. Reducing NH3 emissions is found to be the most effective control strategy for mitigating pNO3 pollution in China. This review suggests that more field measurements are needed to constrain the parameterization of heterogeneous N2O5 and nitrogen dioxide (NO2) uptake. Future studies are also needed to quantify the relationships of pNO3 to AOC, O3, NOx, and volatile organic compounds (VOCs) in different regions of China under different meteorological conditions. Research on multiple-pollutant control strategies involving NH3, NOX, and VOCs is required to mitigate pNO3 pollution, especially during severe winter haze events.

Diagnostic analysis of regional ozone pollution in Yangtze River Delta, China: A case study in summer 2020.

A regional ozone (O3) pollution event occurred in the Yangtze River Delta region during August 17-23, 2020 (except on August 21). This study aims to understand the causes of O3 pollution during the event using an emission-based model (i.e., the Community Multiscale Air Quality (CMAQ) model) and an observation-based model (OBM). The OBM was used to investigate O3 sensitivity to its precursors during the O3 pollution, concluding that O3 formation was limited by volatile organic compounds (VOCs) on August 19, but was co-limited by VOCs and nitrogen oxides (NOx) on other polluted days. Aromatics and alkenes were the two main VOC groups contributing to the O3 formation, with trans-2-butene and m/p-xylene as the key species among the VOCs measured at the Nanjing urban site. The source apportionment results estimated using the source-oriented CMAQ model suggest that the transportation and industry sources dominated the non-background O3 production in Nanjing, which were responsible for 52% and 24.7%, respectively. The O3 concentration attributed to NOx (~70%) was significantly higher than that attributed to VOCs (approximately 30%). The process analysis revealed that vertical mixing increased the O3 concentrations in the early morning, and photochemical reactions promoted O3 formation and accumulation during the daytime within the planetary boundary layer. At night, outflow from horizontal transport and nocturnal chemistry jointly resulted the O3 depletion. The contributions of inter-city transport during the O3 pollution period in Nanjing were also estimated. The predicted O3 concentration was largely recorded from long-distance regions, reaching 46%, followed by local sources (38%) and surrounding cities (16%). The results indicate that both NOx and VOCs contributed significantly to O3 pollution during this event, and the emissions controls of NOx and the key VOC species of aromatics and alkenes from a cooperative regional perspective should be considered to mitigate O3 pollution.

PM2.5 and O3 relationships affected by the atmospheric oxidizing capacity in the Yangtze River Delta, China.

The atmospheric oxidizing capacity (AOC), reflecting the self-cleansing capacity of the atmosphere, plays an important role in the chemical evolution of secondary fine particulate matter (PM2.5) and ozone (O3). In this work, the AOC and its relationships with PM2.5 and O3 were investigated with a chemical transport model (CTM) in the Yangtze River Delta (YRD) region during the four seasons of 2017. The region-wide average AOC is ~4.5×10-4 min-1 in summer and ~ 6.4×10-5 min-1 in winter. Hydroxyl (OH) radicals oxidation contributes 55-69% to the total AOC, followed by nitrate (NO3) radicals and O3 (accounting for 19-34% and < 10%, respectively). The AOC attains a strong positive correlation with the O3 level in all seasons. However, it is weakly or insignificantly correlated with PM2.5 except in summer. Additionally, AOC×(SO2 + NO2 + volatile organic compound (VOC)) is well correlated with the PM2.5 level, and high levels of precursors counteract lower AOC values in cold seasons. Collectively, the results indicate that the abundance of precursors could drive secondary aerosol formation in winter, and aqueous or heterogeneous reactions (not considered in the AOC estimates) are likely of importance at high aerosol loadings in the YRD. The relationship between the daily PM2.5 and O3 levels is affected by the AOC magnitude. PM2.5 and O3 are strongly correlated when the AOC is relatively high, but PM2.5 is independent of O3 under low-AOC (<6.6×10-5 min-1, typically in winter) conditions. This work reveals the dependence of PM2.5-O3 relationships on the AOC, suggesting that joint PM2.5 and O3 reduction could be realized at moderate to high AOC levels, especially in spring and autumn when the cooccurrence of high O3 and PM2.5 events is frequently observed.

Double high pollution events in the Yangtze River Delta from 2015 to 2019: Characteristics, trends, and meteorological situations.

We investigated the spatial distribution and trend of double high pollution (DHP), in which the daily average concentration of fine particulate matter (PM2.5) was above 75 µg/m3 and the daily maximum 8-hour average ozone (MDA8 O3) concentration was above 160 µg/m3, in the Yangtze River Delta (YRD) region during 2015-2019, along with the meteorological and chemical characteristics during DHP and differences compared to high O3 pollution (HOP) and high PM2.5 pollution (HPP). In the YRD, Shanghai had the highest frequency of DHP at 7.6%, while Anhui had the least (2.1%). DHP mostly occurred in the northwest and along the Yangtze River in the east of the YRD, especially in spring (April) and autumn (October). MDA8 O3 level was relatively higher during DHP than HOP, while PM2.5 level was relatively higher during HPP than DHP. In 2015-2019, the total number of DHP events decreased in the YRD, but the changes in PM2.5 and O3 concentrations showed great spatial variations. DHP was often associated with a weak pressure field, under meteorological conditions with east winds, temperatures of 18.7-26.1 °C, relative humidity of 65.7-77.1%, sea level pressure of 1008.2-1019 hPa, wind speed of 1.4-2.4 m/s, and visibility of 3.1-7.5 km. Water-soluble ions (NO3-, NH4+, and SO42-) were the dominant components of PM2.5 during DHP at Nanjing and Changzhou City in 2019. Although the fraction of those ions during DHP and HPP were similar, the secondary conversion of NO2 and SO2 was stronger in HPP. The concentrations of those ions were lowest in HOP, with a higher fraction of sulfate than the other two types of pollution. The conversion of SO2 to sulfate was easier to occur than that of NO2 to nitrate under all the polluted conditions in the two cities.

Effects of using different exposure data to estimate changes in premature mortality attributable to PM2.5 and O3 in China.

The assessment of premature mortality associated with the dramatic changes in fine particulate matter (PM2.5) and ozone (O3) has important scientific significance and provides valuable information for future emission control strategies. Exposure data are particularly vital but may cause great uncertainty in health burden assessments. This study, for the first time, used six methods to generate the concentration data of PM2.5 and O3 in China between 2014 and 2018, and then quantified the changes in premature mortality due to PM2.5 and O3 using the Environmental Benefits Mapping and Analysis Program-Community Edition (BenMAP-CE) model. The results show that PM2.5-related premature mortality in China decreases by 263 (95% confidence interval (CI95): 142-159) to 308 (CI95: 213-241) thousands from 2014 to 2018 by using different concentration data, while O3-related premature mortality increases by 67 (CI95: 26-104) to 103 (CI95: 40-163) thousands. The estimated mean changes are up to 40% different for the PM2.5-related mortality, and up to 30% for the O3-related mortality if different exposure data are chosen. The most significant difference due to the exposure data is found in the areas with a population density of around 103 people/km2, mostly located in Central China, for both PM2.5 and O3. Our results demonstrate that the exposure data source significantly affects mortality estimations and should thus be carefully considered in health burden assessments.

Quantifying the impacts of inter-city transport on air quality in the Yangtze River Delta urban agglomeration, China: Implications for regional cooperative controls of PM2.5 and O3.

The Yangtze River Delta (YRD) urban agglomeration is one of the most developed regions in China. During recent decades, this region has experienced severe regional haze and photochemical smog pollution problems. In this study, we used a source-oriented chemical transport model to quantitatively estimate the effects of inter-city transport on fine particulate matter (PM2.5) and ozone (O3) among the 41 cities in the YRD urban agglomeration during the EXPLORE-YRD (EXPeriment on the eLucidation of the atmospheric Oxidation capacity and aerosol foRmation, and their Effects in the Yangtze River Delta) campaign (May 17 to June 17, 2018). The results show that inter-city transport is very significant in the YRD region. On average, the emissions from the local city, the other YRD cities, and the regions outside of the YRD contribute 25.3%, 49.9%, and 24.8% to the PM2.5, respectively, and they contribute 33.7%, 46.8%, and 19.5% of the non-background O3, respectively. On PM2.5 or O3 pollution days, the transport contribution from the non-local YRD cities becomes much more important, while the local emissions and the transport from non-YRD emissions become less important. The results also suggest that the cities within a distance of 184 km and 94 km contribute 60% of the PM2.5 and O3, respectively. Therefore, we recommend that regional cooperative control programs in the YRD consider emission controls over cities within these ranges. The range for primary PM2.5 (92 km) is very different from that for secondary PM2.5 (515 km). Cooperative emission controls of SO2 and NOx on a much larger regional scale are required to reduce the secondary PM2.5 in the YRD.

Application and evaluation of a low-cost PM sensor and data fusion with CMAQ simulations to quantify the impacts of prescribed burning on air quality in Southwestern Georgia, USA.

Prescribed burning (PB) is a prominent source of PM2.5 in the southeastern US and exposure to PB smoke is a health risk. As demand for burning increases and stricter controls are implemented for other anthropogenic sources, PB emissions tend to be responsible for an increasing fraction of PM2.5 concentrations. Here, to quantify the effect of PB on air quality, low-cost sensors are used to measure PM2.5 concentrations in Southwestern Georgia. The feasibility of using low-cost sensors as a supplemental measurement tool is evaluated by comparing them with reference instruments. A chemical transport model, CMAQ, is also used to simulate the contribution of PB to PM2.5 concentrations. Simulated PM2.5 concentrations are compared to observations from both low-cost sensors and reference monitors. Finally, a data fusion method is applied to generate hourly spatiotemporal exposure fields by fusing PM2.5 concentrations from the CMAQ model and all observations. The results show that the severe impact of PB on local air quality and public health may be missed due to the dearth of regulatory monitoring sites. In Southwestern Georgia PM2.5 concentrations are highly non-homogeneous and the spatial variation is not captured even with a 4-km horizontal resolution in model simulations. Low-cost PM sensors can improve the detection of PB impacts and provide useful spatial and temporal information for integration with air quality models. R2 of regression with observations increases from an average of 0.09 to 0.40 when data fusion is applied to model simulation withholding the observations at the evaluation site. Adding observations from low-cost sensors reduces the underestimation of nighttime PM2.5 concentrations and reproduces the peaks that are missed by the simulations. In the future, observations from a dense network of low-cost sensors could be fused with the model simulated PM2.5 fields to provide better estimates of hourly exposures to smoke from PB.Implications: Prescribed burning emissions are a major cause of elevated PM2.5 concentrations, posing a risk to human health. However, their impact cannot be quantified properly due to a dearth of regulatory monitoring sites in certain regions of the United States such as Southwestern Georgia. Low-cost PM sensors can be used as a supplemental measurement tool and provide useful spatial and temporal information for integration with air quality model simulations. In the future, data from a dense network of low-cost sensors could be fused with model simulated PM2.5 fields to provide improved estimates of hourly exposures to smoke from prescribed burning.

Modeling secondary organic aerosol formation from volatile chemical products.

Volatile chemical products (VCPs) are commonly-used consumer and industrial items that are an important source of anthropogenic emissions. Organic compounds from VCPs evaporate on atmospherically relevant time scales and include many species that are secondary organic aerosol (SOA) precursors. However, the chemistry leading to SOA, particularly that of intermediate volatility organic compounds (IVOCs), has not been fully represented in regional-scale models such as the Community Multiscale Air Quality (CMAQ) model, which tend to underpredict SOA concentrations in urban areas. Here we develop a model to represent SOA formation from VCP emissions. The model incorporates a new VCP emissions inventory and employs three new classes of emissions: siloxanes, oxygenated IVOCs, and nonoxygenated IVOCs. VCPs are estimated to produce 1.67 µg m-3 of noontime SOA, doubling the current model predictions and reducing the SOA mass concentration bias from -75% to -58% when compared to observations in Los Angeles in 2010. While oxygenated and nonoxygenated intermediate volatility VCP species are emitted in similar quantities, SOA formation is dominated by the nonoxygenated IVOCs. Formaldehyde and SOA show similar relationships to temperature and bias signatures indicating common sources and/or chemistry. This work suggests that VCPs contribute up to half of anthropogenic SOA in Los Angeles and models must better represent SOA precursors from VCPs to predict the urban enhancement of SOA.

Criteria pollutant impacts of volatile chemical products informed by near-field modeling.

Consumer, industrial, and commercial product usage is a source of exposure to potentially hazardous chemicals. In addition, cleaning agents, personal care products, coatings, and other volatile chemical products (VCPs), evaporate and react in the atmosphere producing secondary pollutants. Here, we show high air emissions from VCP usage (≥ 14 kg person-1 yr-1, at least 1.7× higher than current operational estimates) are supported by multiple estimation methods and constraints imposed by ambient levels of ozone, hydroxyl radical (OH) reactivity, and the organic component of fine particulate matter (PM2.5) in Pasadena, California. A near-field model, which estimates human chemical exposure during or in the vicinity of product use, indicates these high air emissions are consistent with organic product usage up to ~75 kg person-1 yr-1, and inhalation of consumer products could be a non-negligible exposure pathway. After constraining the PM2.5 yield to 5% by mass, VCPs produce ~41% of the photochemical organic PM2.5 (1.1 ± 0.3 µg m-3) and ~17% of maximum daily 8-hr average ozone (9 ± 2 ppb) in summer Los Angeles. Therefore, both toxicity and ambient criteria pollutant formation should be considered when organic substituents are developed for VCPs in pursuit of safer and sustainable products and cleaner air.

Simulation of organic aerosol formation during the CalNex study: updated mobile emissions and secondary organic aerosol parameterization for intermediate-volatility organic compounds.

We describe simulations using an updated version of the Community Multiscale Air Quality model version 5.3 (CMAQ v5.3) to investigate the contribution of intermediate-volatility organic compounds (IVOCs) to secondary organic aerosol (SOA) formation in southern California during the CalNex study. We first derive a model-ready parameterization for SOA formation from IVOC emissions from mobile sources. To account for SOA formation from both diesel and gasoline sources, the parameterization has six lumped precursor species that resolve both volatility and molecular structure (aromatic versus aliphatic). We also implement new mobile-source emission profiles that quantify all IVOCs based on direct measurements. The profiles have been released in SPECIATE 5.0. By incorporating both comprehensive mobile-source emission profiles for semivolatile organic compounds (SVOCs) and IVOCs and experimentally constrained SOA yields, this CMAQ configuration best represents the contribution of mobile sources to urban and regional ambient organic aerosol (OA). In the Los Angeles region, gasoline sources emit 4 times more non-methane organic gases (NMOGs) than diesel sources, but diesel emits roughly 3 times more IVOCs on an absolute basis. The revised model predicts all mobile sources (including on- and off-road gasoline, aircraft, and on- and off-road diesel) contribute ~ 1 µgm-3 to the daily peak SOA concentration in Pasadena. This represents a ~ 70% increase in predicted daily peak SOA formation compared to the base version of CMAQ. Therefore, IVOCs in mobile-source emissions contribute almost as much SOA as traditional precursors such as single-ring aromatics. However, accounting for these emissions in CMAQ does not reproduce measurements of either ambient SOA or IVOCs. To investigate the potential contribution of other IVOC sources, we performed two exploratory simulations with varying amounts of IVOC emissions from nonmobile sources. To close the mass balance of primary hydrocarbon IVOCs, IVOCs would need to account for 12% of NMOG emissions from nonmobile sources (or equivalently 30.7 t d-1 in the Los Angeles-Pasadena region), a value that is well within the reported range of IVOC content from volatile chemical products. To close the SOA mass balance and also explain the mildly oxygenated IVOCs in Pasadena, an additional 14.8% of nonmobile-source NMOG emissions would need to be IVOCs (assuming SOA yields from the mobile IVOCs apply to nonmobile IVOCs). However, an IVOC-to-NMOG ratio of 26.8% (or equivalently 68.5 t d-1 in the Los Angeles-Pasadena region) for nonmobile sources is likely unrealistically high. Our results highlight the important contribution of IVOCs to SOA production in the Los Angeles region but underscore that other uncertainties must be addressed (multigenerational aging, aqueous chemistry and vapor wall losses) to close the SOA mass balance. This research also highlights the effectiveness of regulations to reduce mobile-source emissions, which have in turn increased the relative importance of other sources, such as volatile chemical products.

Driving Forces of Changes in Air Quality during the COVID-19 Lockdown Period in the Yangtze River Delta Region, China.

During the COVID-19 lockdown period (from January 23 to February 29, 2020), ambient PM2.5 concentrations in the Yangtze River Delta (YRD) region were observed to be much lower, while the maximum daily 8 h average (MDA8) O3 concentrations became much higher compared to those before the lockdown (from January 1 to 22, 2020). Here, we show that emission reduction is the major driving force for the PM2.5 change, contributing to a PM2.5 decrease by 37% to 55% in the four YRD major cities (i.e., Shanghai, Hangzhou, Nanjing, and Hefei), but the MDA8 O3 increase is driven by both emission reduction (29%-52%) and variation in meteorological conditions (17%- 49%). Among all pollutants, reduction in emissions mainly of primary PM contributes to a PM2.5 decrease by 28% to 46%, and NOx emission reduction contributes 7% to 10%. Although NOx emission reduction dominates the MDA8 O3 increase (38%-59%), volatile organic compounds (VOCs) emission reduction lead to a 5% to 9% MDA8 O3 decrease. Increased O3 promotes secondary aerosol formation and partially offsets the decrease of PM2.5 caused by the primary PM emission reductions. The results demonstrate that more coordinated air pollution control strategies are needed in YRD.

Drought Impacts on Secondary Organic Aerosol: A Case Study in the Southeast United States.

Secondary organic aerosol (SOA) is a significant component of fine particulate matter, and it has increased during past drought periods in the U.S. Here, we use the Community Multiscale Air Quality (CMAQ) model to characterize the complex effects of drought on SOA through a case study comparing a drought period (June 2011) and a wet period (June 2013) over the southeast U.S. The model simulates a 68% (1.7 µg/m3) higher SOA concentration at the surface during drought and attributes 98% of this increase to biogenic SOA. Through model sensitivity simulations, the SOA increase associated with drought is attributed to 54% from accelerated gas-phase reactions oxidizing volatile organic compounds (VOCs) to SOA, 45% from higher emissions of biogenic VOCs, 18% from enhanced acid-catalyzed production of isoprene SOA in aerosol water due to changing sulfate, 3% from enhanced in-cloud aqueous phase chemistry. Because the higher SOA levels overwhelm the reduced precipitation, there is an increase in wet deposition flux in the drought month which offsets 20% of the total SOA increase. If anthropogenic emissions are held constant, anthropogenic SOA is 51% higher during drought, highlighting the importance of meteorological impacts on chemistry.

Atmospheric PAHs in North China: Spatial distribution and sources.

Polycyclic aromatic hydrocarbons (PAHs), formed through incomplete combustion process, have adverse health effects. To investigate spatial distribution and sources of PAHs in North China, PAHs with passive sampling in 90 gridded sites during June to September in 2011 were analyzed. The average concentration of the sum of fifteen PAHs in North China is 220±14ng/m(3), with the highest in Shanxi, followed by Shandong and Hebei, and then the Beijing-Tianjin area. Major sources of PAHs are identified for each region of North China, coke process for Shanxi, biomass burning for Hebei and Shandong, and coal combustion for Beijing-Tianjin area, respectively. Emission inventory is combined with back trajectory analysis to study the influence of emissions from surrounding areas at receptor sites. Shanxi and Beijing-Tianjin areas are more influenced by sources nearby while regional sources have more impact on Hebei and Shandong areas. Results from this study suggest the areas where local emission should be the major target for control and areas where both local and regional sources should be considered for PAH abatement in North China.