Predicting the climate impact of aviation for en-route emissions: the algorithmic climate change function submodel ACCF 1.0 of EMAC 2.53

Using climate-optimized flight trajectories is one essential measure to reduce aviation's climate impact. Detailed knowledge of temporal and spatial climate sensitivity for aviation emissions in the atmosphere is required to realize such a climate mitigation measure. The algorithmic Climate Change Functions (aCCFs) represent the basis for such purposes. This paper presents the first version of the Algorithmic Climate Change Function submodel (ACCF 1.0) within the European Centre HAMburg general circulation model (ECHAM) and Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model framework. In the ACCF 1.0, we implement a set of aCCFs (version 1.0) to estimate the average temperature response over 20 years (ATR20) resulting from aviation CO2 emissions and non-CO2 impacts, such as NOx emissions (via ozone production and methane destruction), water vapour emissions, and contrail cirrus. While the aCCF concept has been introduced in previous research, here, we publish a consistent set of aCCF formulas in terms of fuel scenario, metric, and efficacy for the first time. In particular, this paper elaborates on contrail aCCF development, which has not been published before. ACCF 1.0 uses the simulated atmospheric conditions at the emission location as input to calculate the ATR20 per unit of fuel burned, per NOx emitted, or per flown kilometre.In this research, we perform quality checks of the ACCF 1.0 outputs in two aspects. Firstly, we compare climatological values calculated by ACCF 1.0 to previous studies. The comparison confirms that in the Northern Hemisphere between 150–300 hPa altitude (flight corridor), the vertical and latitudinal structure of NOx-induced ozone and H2O effects are well represented by the ACCF model output. The NOx-induced methane effects increase towards lower altitudes and higher latitudes, which behaves differently from the existing literature. For contrail cirrus, the climatological pattern of the ACCF model output corresponds with the literature, except that contrail-cirrus aCCF generates values at low altitudes near polar regions, which is caused by the conditions set up for contrail formation. Secondly, we evaluate the reduction of NOx-induced ozone effects through trajectory optimization, employing the tagging chemistry approach (contribution approach to tag species according to their emission categories and to inherit these tags to other species during the subsequent chemical reactions). The simulation results show that climate-optimized trajectories reduce the radiative forcing contribution from aviation NOx-induced ozone compared to cost-optimized trajectories. Finally, we couple the ACCF 1.0 to the air traffic simulation submodel AirTraf version 2.0 and demonstrate the variability of the flight trajectories when the efficacy of individual effects is considered. Based on the 1 d simulation results of a subset of European flights, the total ATR20 of the climate-optimized flights is significantly lower (roughly 50 % less) than that of the cost-optimized flights, with the most considerable contribution from contrail cirrus. The CO2 contribution observed in this study is low compared with the non-CO2 effects, which requires further diagnosis.

Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation

The unprecedented lockdown of human activities during the COVID-19 pandemic has significantly influenced social life in China. However, understanding the impact of this unique event on the emissions of different species is still insufficient, prohibiting the proper assessment of the environmental impacts of COVID-19 restrictions. Here we developed a multi-air-pollutant inversion system to simultaneously estimate the emissions of NOx, SO2, CO, PM2.5 and PM10 in China during COVID-19 restrictions with high temporal (daily) and horizontal (15 km) resolutions. Subsequently, contributions of emission changes versus meteorological variations during the COVID-19 lockdown were separated and quantified. The results demonstrated that the inversion system effectively reproduced the actual emission variations in multi-air pollutants in China during different periods of COVID-19 lockdown, which indicate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing substantially by ∼40 %. However, emissions of other air pollutants were found to only decrease by∼10% because power generation and heavy industrial processes were not halted during lockdown, and residential activities may actually have increased due to the stay-at-home orders. Consequently, although obvious reductions of PM2.5 concentrations occurred over the North China Plain (NCP) during the lockdown period, the emission change only accounted for 8.6 % of PM2.5 reductions and even led to substantial increases in O3. The meteorological variation instead dominated the changes in PM2.5 concentrations over the NCP, which contributed 90 % of the PM2.5 reductions over most parts of the NCP region. Meanwhile, our results suggest that the local stagnant meteorological conditions, together with inefficient reductions of PM2.5 emissions, were the main drivers of the unexpected PM2.5 pollution in Beijing during the lockdown period. These results highlighted that traffic control as a separate pollution control measure has limited effects on the coordinated control of O3 and PM2.5 concentrations under current complex air pollution conditions in China. More comprehensive and balanced regulations for multiple precursors from different sectors are required to address O3 and PM2.5 pollution in China.

Two years of volatile organic compound online in situ measurements at the Site Instrumental de Recherche par Télédétection Atmosphérique (Paris region, France) using proton-transfer-reaction mass spectrometry

Volatile organic compounds (VOCs) have direct influences on air quality and climate. They indeed play a key role in atmospheric chemistry as precursors of secondary pollutants, such as ozone (O3) and secondary organic aerosols (SOA). In this respect, long-term datasets of in situ atmospheric measurements are crucial for characterizing the variability of atmospheric chemical composition, its sources, and trends. The ongoing establishment of the Aerosols, Cloud, and Trace gases Research InfraStructure (ACTRIS) allows implementation of the collection and provision of such high-quality datasets. In this context, online and continuous measurements of O3, nitrogen oxides (NOx), and aerosols have been carried out since 2012 at the SIRTA (Site Instrumental de Recherche par Télédétection Atmosphérique) observatory, located in the Paris region, France. Within the last decade, VOC measurements were conducted offline at SIRTA, until the implementation of real-time monitoring which started in January 2020 using a proton-transfer-reaction quadrupole mass spectrometer (PTR-Q-MS).The dataset acquired during the first 2 years of online VOC measurements provides insights into their seasonal and diurnal variabilities. The additional long-term datasets obtained from co-located measurements (NOx, aerosol physical and chemical properties, meteorological parameters) are used to better characterize the atmospheric conditions and to further interpret the obtained results. Results also include insights into VOC main sources and the influence of meteorological conditions and air mass origin on their levels in the Paris region. Due to the COVID-19 pandemic, the year 2020 notably saw a quasi-total lockdown in France in spring and a lighter one in autumn. Therefore, the focus is placed on the impact of these lockdowns on the VOC variability and sources. A change in the behaviour of VOC markers for anthropogenic sources was observed during the first lockdown, reflecting a change in human activities. A comparison with gas chromatography data from the Paris city centre consolidates the regional representativity of the SIRTA station for benzene, while differences are observed for shorter-lived compounds with a notable impact of their local sources. This dataset could be further used as input for atmospheric models and can be found at 10.14768/f8c46735-e6c3-45e2-8f6f-26c6d67c4723 (Simon et al., 2022a).

Estimation of NO2 emission strengths over Riyadh and Madrid from space from a combination of wind-assigned anomalies and a machine learning technique

Nitrogen dioxide (NO2) air pollution provides valuable information for quantifying NOx (NOx = NO + NO2) emissions and exposures. This study presents a comprehensive method to estimate average tropospheric NO2 emission strengths derived from 4-year (May 2018–June 2022) TROPOspheric Monitoring Instrument (TROPOMI) observations by combining a wind-assigned anomaly approach and a machine learning (ML) method, the so-called gradient descent algorithm. This combined approach is firstly applied to the Saudi Arabian capital city of Riyadh, as a test site, and yields a total emission rate of 1.09×1026 molec. s-1. The ML-trained anomalies fit very well with the wind-assigned anomalies, with an R2 value of 1.0 and a slope of 0.99. Hotspots of NO2 emissions are apparent at several sites: over a cement plant and power plants as well as over areas along highways. Using the same approach, an emission rate of 1.99×1025 molec. s-1 is estimated in the Madrid metropolitan area, Spain. Both the estimate and spatial pattern are comparable with the Copernicus Atmosphere Monitoring Service (CAMS) inventory.Weekly variations in NO2 emission are highly related to anthropogenic activities, such as the transport sector. The NO2 emissions were reduced by 16 % at weekends in Riyadh, and high reductions were found near the city center and in areas along the highway. An average weekend reduction estimate of 28 % was found in Madrid. The regions with dominant sources are located in the east of Madrid, where residential areas and the Madrid-Barajas airport are located. Additionally, due to the COVID-19 lockdowns, the NO2 emissions decreased by 21 % in March–June 2020 in Riyadh compared with the same period in 2019. A much higher reduction (62 %) is estimated for Madrid, where a very strict lockdown policy was implemented. The high emission strengths during lockdown only persist in the residential areas, and they cover smaller areas on weekdays compared with weekends. The spatial patterns of NO2 emission strengths during lockdown are similar to those observed at weekends in both cities. Although our analysis is limited to two cities as test examples, the method has proven to provide reliable and consistent results. It is expected to be suitable for other trace gases and other target regions. However, it might become challenging in some areas with complicated emission sources and topography, and specific NO2 decay times in different regions and seasons should be taken into account. These impacting factors should be considered in the future model to further reduce the uncertainty budget.

Potential of TROPOMI for understanding spatio-temporal variations in surface NO2 and their dependencies upon land use over the Iberian Peninsula

In orbit since late 2017, the Tropospheric Monitoring Instrument (TROPOMI) is offering new outstanding opportunities for better understanding the emission and fate of nitrogen dioxide (NO2) pollution in the troposphere. In this study, we provide a comprehensive analysis of the spatio-temporal variability of TROPOMI NO2 tropospheric columns (TrC-NO2) over the Iberian Peninsula during 2018–2021, considering the recently developed Product Algorithm Laboratory (PAL) product. We complement our analysis with estimates of NOx anthropogenic and natural soil emissions. Closely related to cloud cover, the data availability of TROPOMI observations ranges from 30 %–45 % during April and November to 70 %–80 % during summertime, with strong variations between northern and southern Spain. Strongest TrC-NO2 hotspots are located over Madrid and Barcelona, while TrC-NO2 enhancements are also observed along international maritime routes close the strait of Gibraltar, and to a lesser extent along specific major highways. TROPOMI TrC-NO2 appear reasonably well correlated with collocated surface NO2 mixing ratios, with correlations around 0.7–0.8 depending on the averaging time.We investigate the changes of weekly and monthly variability of TROPOMI TrC-NO2 depending on the urban cover fraction. Weekly profiles show a reduction of TrC-NO2 during the weekend ranging from -10 % to -40 % from least to most urbanized areas, in reasonable agreement with surface NO2. In the largest agglomerations like Madrid or Barcelona, this weekend effect peaks not in the city center but in specific suburban areas/cities, suggesting a larger relative contribution of commuting to total NOx anthropogenic emissions. The TROPOMI TrC-NO2 monthly variability also strongly varies with the level of urbanization, with monthly differences relative to annual mean ranging from -40 % in summer to +60 % in winter in the most urbanized areas, and from -10 % to +20 % in the least urbanized areas. When focusing on agricultural areas, TROPOMI observations depict an enhancement in June–July that could come from natural soil NO emissions. Some specific analysis of surface NO2 observations in Madrid show that the relatively sharp NO2 minimum used to occur in August (drop of road transport during holidays) has now evolved into a much broader minimum partly de-coupled from the observed local road traffic counting;this change started in 2018, thus before the COVID-19 outbreak. Over 2019–2021, a reasonable consistency of the inter-annual variability of NO2 is also found between both datasets.Our study illustrates the strong potential of TROPOMI TrC-NO2 observations for complementing the existing surface NO2 monitoring stations, especially in the poorly covered rural and maritime areas where NOx can play a key role, notably for the production of tropospheric O3.

Pandemic restrictions in 2020 highlight the significance of non-road NOx sources in central London

Fluxes of nitrogen oxides (NOx=NO+NO2) and carbon dioxide (CO2) were measured using eddy covariance at the British Telecommunications (BT) Tower in central London during the coronavirus pandemic. Comparing fluxes to those measured in 2017 prior to the pandemic restrictions and the introduction of the Ultra-Low Emissions Zone (ULEZ) highlighted a 73 % reduction in NOx emissions between the two periods but only a 20 % reduction in CO2 emissions and a 32 % reduction in traffic load. Use of a footprint model and the London Atmospheric Emissions Inventory (LAEI) identified transport and heat and power generation to be the two dominant sources of NOx and CO2 but with significantly different relative contributions for each species. Application of external constraints on NOx and CO2 emissions allowed the reductions in the different sources to be untangled, identifying that transport NOx emissions had reduced by >73 % since 2017. This was attributed in part to the success of air quality policy in central London but crucially due to the substantial reduction in congestion that resulted from pandemic-reduced mobility. Spatial mapping of the fluxes suggests that central London was dominated by point source heat and power generation emissions during the period of reduced mobility. This will have important implications on future air quality policy for NO2 which, until now, has been primarily focused on the emissions from diesel exhausts.

Air quality changes in Taiwan over the past decades and during the COVID-19 crisis

Over the past decades, Taiwan has achieved remarkable goals in air pollution reduction with the concentrations of several common air pollutants such as CO, NOx, PM10, PM2.5, and SO2 going down. In contrast to these achievements, the mitigation of O3 remains extremely tough due to the complexity of its formation process involving synergistic effects of precursor reductions and meteorological influences. During the local COVID-19 crises in Taiwan and the Level 3 alert in 2021, air pollutants directly emitted from the traffic such as CO and NOx present clear relationships with the drop of the recorded freeway traffic volume due to the alert, while PM10 and PM2.5 which are also relevant to the traffic do not show indications of being greatly influenced by the decrease of the traffic flow. Although road traffic is not regarded as a main source of SO2 by current understanding, the unusual SO2 variation patterns found in this study suggest a prolonged impact for months from the changes of travel behavior during the epidemic. In contrast, the epidemic did not exert influences on industrial SO2 concentration which accounts for a large portion of total SO2 in Taiwan, and a similar scenario is also seen in each type of O3 monitoring. Although some results discussed in this study are not in line with current consensuses and understandings in terms of the nation of certain air pollutants, these findings may disclose new perspectives which could be a potential benefit to air quality improvement projects in the future.

Changing ozone sensitivity in the South Coast Air Basin during the COVID-19 period

The South Coast Air Basin (SoCAB), which includes the city of Los Angeles and is home to more than 15 million people, frequently experiences ozone (O3) levels that exceed ambient air quality standards. While strict regulation of O3 precursors has dramatically improved air quality over the past 50 years, the region has seen limited improvement in O3 over the past decade despite continued reductions in precursor emissions. One contributing factor to the recent lack of improvement is a gradual transition of the underlying photochemical environment from a VOC-limited regime (where VOC denotes volatile organic compound) towards an NOx-limited one. The changes in human activity prompted by COVID-19-related precautions in spring and summer of 2020 exacerbated these existing changes in the O3 precursor environment. Analyses of sector-wide changes in activity indicate that emissions of NOx decreased by 15 %–20 % during spring (April–May) and by 5 %–10 % during summer (June–July) relative to expected emissions for 2020, largely due to changes in mobile-source activity. Historical trend analysis from two indicators of O3 sensitivity (the satellite HCHO/NO2 ratio and the O3 weekend/weekday ratio) revealed that spring of 2020 was the first year on record to be on averageNOx-limited, while the “transitional” character of recent summers became NOx-limited due to COVID-19-related NOx reductions in 2020. Model simulations performed with baseline and COVID-19-adjusted emissions capture this change to an NOx-limited environment and suggest that COVID-19-related emission reductions were responsible for a 0–2 ppb decrease in O3 over the study period. Reaching NOx-limited territory is an important regulatory milestone, and this study suggests that deep reductions in NOx emissions (in excess of those observed in this study) would be an effective pathway toward long-term O3 reductions.

The effect of COVID-19 restrictions on atmospheric new particle formation in Beijing

During the COVID-19 lockdown, the dramatic reduction of anthropogenic emissions provided a unique opportunity to investigate the effects of reduced anthropogenic activity and primary emissions on atmospheric chemical processes and the consequent formation of secondary pollutants. Here, we utilize comprehensive observations to examine the response of atmospheric new particle formation (NPF) to the changes in the atmospheric chemical cocktail. We find that the main clustering process was unaffected by the drastically reduced traffic emissions, and the formation rate of 1.5 nm particles remained unaltered. However, particle survival probability was enhanced due to an increased particle growth rate (GR) during the lockdown period, explaining the enhanced NPF activity in earlier studies. For GR at 1.5–3 nm, sulfuric acid (SA) was the main contributor at high temperatures, whilst there were unaccounted contributing vapors at low temperatures. For GR at 3–7 and 7–15 nm, oxygenated organic molecules (OOMs) played a major role. Surprisingly, OOM composition and volatility were insensitive to the large change of atmospheric NOx concentration;instead the associated high particle growth rates and high OOM concentration during the lockdown period were mostly caused by the enhanced atmospheric oxidative capacity. Overall, our findings suggest a limited role of traffic emissions in NPF.

Evaluating NOx emissions and their effect on O3 production in Texas using TROPOMI NO2 and HCHO

The Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite is a valuable source of information to monitor the NOx emissions that adversely affect air quality. We conduct a series of experiments using a 4×4 km2 Comprehensive Air Quality Model with Extensions (CAMx) simulation during April–September 2019 in eastern Texas to evaluate the multiple challenges that arise from reconciling the NOx emissions in model simulations with TROPOMI. We find an increase in NO2 (+17 % in urban areas) when transitioning from the TROPOMI NO2 version 1.3 algorithm to the version 2.3.1 algorithm in eastern Texas, with the greatest difference (+25 %) in the city centers and smaller differences (+5 %) in less polluted areas. We find that lightningNOx emissions in the model simulation contribute up to 24 % of the column NO2 in the areas over the Gulf of Mexico and 8% in Texas urban areas. NOx emissions inventories, when using locally resolved inputs, agree with NOx emissions derived from TROPOMI NO2 version 2.3.1 to within 20 % in most circumstances, with a small NOx underestimate in Dallas–Fort Worth (-13 %) and Houston (-20 %). In the vicinity of large power plant plumes (e.g., Martin Lake and Limestone) we find larger disagreements, i.e., the satellite NO2 is consistently smaller by 40 %–60 % than the modeled NO2, which incorporates measured stack emissions. We find that TROPOMI is having difficulty distinguishingNO2 attributed to power plants from the background NO2 concentrations in Texas – an area with atmospheric conditions that cause short NO2 lifetimes. Second, the NOx/NO2 ratio in the model may be underestimated due to the 4 km grid cell size. To understand ozone formation regimes in the area, we combine NO2 column information with formaldehyde (HCHO) column information. We find modest low biases in the model relative to TROPOMI HCHO, with -9 % underestimate in eastern Texas and -21 % in areas of central Texas with lower biogenic volatile organic compound (VOC) emissions. Ozone formation regimes at the time of the early afternoon overpass are NOx limited almost everywhere in the domain, except along the Houston Ship Channel, near the Dallas/Fort Worth International airport, and in the presence of undiluted power plant plumes. There are likely NOx-saturated ozone formation conditions in the early morning hours that TROPOMI cannot observe and would be well-suited for analysis with NO2 and HCHO from the upcoming TEMPO (Tropospheric Emissions: Monitoring Pollution) mission. This study highlights that TROPOMI measurements offer a valuable means to validate emissions inventories and ozone formation regimes, with important limitations.

Environmental Geochemistry and Positive Impact of Covid-19 Pandemic with Special Emphasis to Coal Mining Industry: An Overview

In the present situation, Covid-19 is considered to be an unbeaten global pandemic. In every single fleeting moment, this SARS-CoV-2 (coronavirus-2) causes greater damage to our life including the physical world including drastic imbalance of the whole economic condition of any country. The lockdown governed in two consecutive years (2020 and 2021) in the world to control the spreading of the virus poses an undue threat to the industrial sectors including the coal mining sectors that determine the economic growth of the country. With these negative impacts of coronavirus-2 in our life, this present review aims to explore some of the positive influences of the Covid-19 pandemic through the restoration of the environmental system which are otherwise not possible. This quantitative review finds that spreading of the Covid-19 pandemic indirectly improves the air and water quality by reducing the number of vehicles, reduces the CO2, NOx, particulate matter, and other polluting gases emission from coal-based power plants through periodical lockdown in the country. Moreover, the lockdown implemented to minimise the spreading of the Covid-19 significantly reduces the coal dust production from the mining and transportation of coal that indirectly reduces environmental pollution.

European primary emissions of criteria pollutants and greenhouse gases in 2020 modulated by the COVID-19 pandemic disruptions

We present a European dataset of daily sector-, pollutant- and country-dependent emission adjustment factors associated with the COVID-19 mobility restrictions for the year 2020. We considered metrics traditionally used to estimate emissions, such as energy statistics or traffic counts, as well as information derived from new mobility indicators and machine learning techniques. The resulting dataset covers a total of nine emission sectors, including road transport, the energy industry, the manufacturing industry, residential and commercial combustion, aviation, shipping, off-road transport, use of solvents, and fugitive emissions from transportation and distribution of fossil fuels. The dataset was produced to be combined with the Copernicus CAMS-REG_v5.1 2020 business-as-usual (BAU) inventory, which provides high-resolution (0.1∘×0.05∘) emission estimates for 2020 omitting the impact of the COVID-19 restrictions. The combination of both datasets allows quantifying spatially and temporally resolved reductions in primary emissions from both criteria pollutants (NOx, SO2, non-methane volatile organic compounds – NMVOCs, NH3, CO, PM10 and PM2.5) and greenhouse gases (CO2 fossil fuel, CO2 biofuel andCH4), as well as assessing the contribution of each emission sector and European country to the overall emission changes. Estimated overall emission changes in 2020 relative to BAU emissions were as follows: -10.5 % forNOx (-602 kt), -7.8 % (-260.2 Mt) for CO2 from fossil fuels,-4.7 % (-808.5 kt) for CO, -4.6 % (-80 kt) for SO2, -3.3 % (-19.1 Mt) for CO2 from biofuels, -3.0 % (-56.3 kt) for PM10, -2.5 % (-173.3 kt) for NMVOCs, -2.1 % (-24.3 kt) for PM2.5, -0.9 % (-156.1 kt) for CH4 and -0.2 % (-8.6 kt) for NH3. The most pronounced drop in emissions occurred in April (up to -32.8 % on average forNOx) when mobility restrictions were at their maxima. The emission reductions during the second epidemic wave between October and December were 3 to 4 times lower than those occurred during the spring lockdown, as mobility restrictions were generally softer (e.g. curfews, limited social gatherings). Italy, France, Spain, the United Kingdom and Germany were, together, the largest contributors to the total EU27 + UK (27 member states of the European Union and the UK) absolute emission decreases. At the sectoral level, the largest emission declines were found for aviation (-51 % to -56 %), followed by road transport (-15.5 % to -18.8 %), the latter being the main driver of the estimated reductions for the majority of pollutants. The collection of COVID-19 emission adjustment factors (10.24380/k966-3957, Guevara et al., 2022) and the CAMS-REG_v5.1 2020 BAU gridded inventory (10.24380/eptm-kn40, Kuenen et al., 2022b) have been produced in support of air quality modelling studies.

Secondary PM2.5 decreases significantly less than NO2 emission reductions during COVID lockdown in Germany

This study estimates the influence of anthropogenic emission reductions on the concentration of particulate matter with a diameter smaller than 2.5 µm (PM2.5) during the 2020 lockdown period in German metropolitan areas. After accounting for meteorological effects, PM2.5 concentrations during the spring 2020 lockdown period were 5 % lower compared to the same time period in 2019. However, during the 2020 pre-lockdown period (winter), PM2.5 concentrations with meteorology accounted for were 19 % lower than in 2019. Meanwhile, NO2 concentrations with meteorology accounted for dropped by 23 % during the 2020 lockdown period compared to an only 9 % drop for the 2020 pre-lockdown period, both compared to 2019. SO2 and CO concentrations with meteorology accounted for show no significant changes during the 2020 lockdown period compared to 2019. GEOS-Chem (GC) simulations with a COVID-19 emission reduction scenario based on the observations (23 % reduction in anthropogenic NOx emission with unchanged anthropogenic volatile organic compounds (VOCs) and SO2) are consistent with the small reductions of PM2.5 during the lockdown and are used to identify the underlying drivers for this. Due to being in a NOx-saturated ozone production regime, GC OH radical and O3 concentrations increased (15 % and 9 %, respectively) during the lockdown compared to a business-as-usual (BAU, no lockdown) scenario. Ox (equal to NO2+O3) analysis implies that the increase in ozone at nighttime is solely due to reduced NO titration. The increased O3 results in increased NO3 radical concentrations, primarily during the night, despite the large reductions in NO2. Thus, the oxidative capacity of the atmosphere is increased in all three important oxidants, OH, O3, and NO3. PM nitrate formation from gas-phase nitric acid (HNO3) is decreased during the lockdown as the increased OH concentration cannot compensate for the strong reductions in NO2, resulting in decreased daytime HNO3 formation from the OH + NO2 reaction. However, nighttime formation of PM nitrate from N2O5 hydrolysis is relatively unchanged. This results from the fact that increased nighttime O3 results in significantly increased NO3, which roughly balances the effect of the strong NO2 reductions on N2O5 formation. Ultimately, the only small observed decrease in lockdown PM2.5 concentrations can be explained by the large contribution of nighttime PM nitrate formation, generally enhanced sulfate formation, and slightly decreased ammonium. This study also suggests that high PM2.5 episodes in early spring are linked to high atmospheric ammonia concentrations combined with favorable meteorological conditions of low temperature and low boundary layer height. Northwest Germany is a hot-spot of NH3 emissions, primarily emitted from livestock farming and intensive agricultural activities (fertilizer application), with high NH3 concentrations in the early spring and summer months. Based on our findings, we suggest that appropriate NOx and VOC emission controls are required to limit ozone, and that should also help reduce PM2.5. Regulation of NH3 emissions, primarily from agricultural sectors, could result in significant reductions in PM2.5 pollution.

Trends in secondary inorganic aerosol pollution in China and its responses to emission controls of precursors in wintertime

The Chinese government recently proposed ammonia (NH3) emission reductions (but without a specific national target) as a strategic option to mitigate fine particulate matter (PM2.5) pollution. We combined a meta-analysis of nationwide measurements and air quality modeling to identify efficiency gains by striking a balance between controlling NH3 and acid gas (SO2 and NOx) emissions. We found that PM2.5 concentrations decreased from 2000 to 2019, but annual mean PM2.5 concentrations still exceeded 35 µg m-3 at 74 % of 1498 monitoring sites during 2015–2019. The concentration of PM2.5 and its components were significantly higher (16 %–195 %) on hazy days than on non-hazy days. Compared with mean values of other components, this difference was more significant for the secondary inorganic ions SO42-, NO3-, and NH4+ (average increase 98 %). While sulfate concentrations significantly decreased over this period, no significant change was observed for nitrate and ammonium concentrations. Model simulations indicate that the effectiveness of a 50 % NH3 emission reduction for controlling secondary inorganic aerosol (SIA) concentrations decreased from 2010 to 2017 in four megacity clusters of eastern China, simulated for the month of January under fixed meteorological conditions (2010). Although the effectiveness further declined in 2020 for simulations including the natural experiment of substantial reductions in acid gas emissions during the COVID-19 pandemic, the resulting reductions in SIA concentrations were on average 20.8 % lower than those in 2017. In addition, the reduction in SIA concentrations in 2017 was greater for 50 % acid gas reductions than for the 50 % NH3 emission reductions. Our findings indicate that persistent secondary inorganic aerosol pollution in China is limited by emissions of acid gases, while an additional control of NH3 emissions would become more important as reductions of SO2 and NOx emissions progress.

Tropospheric ozone production and chemical regime analysis during the COVID-19 lockdown over Europe

The COVID-19 (coronavirus disease 2019) European lockdowns have led to a significant reduction in the emissions of primary pollutants such as NO (nitric oxide) and NO2 (nitrogen dioxide). As most photochemical processes are related to nitrogen oxide (NOx≡ NO + NO2) chemistry, this event has presented an exceptional opportunity to investigate its effects on air quality and secondary pollutants, such as tropospheric ozone (O3). In this study, we present the effects of the COVID-19 lockdown on atmospheric trace gas concentrations, net ozone production rates (NOPRs) and the dominant chemical regime throughout the troposphere based on three different research aircraft campaigns across Europe. These are the UTOPIHAN (Upper Tropospheric Ozone: Processes Involving HOx and NOx) campaigns in 2003 and 2004, the HOOVN1 -https://media.proquest.com/media/hms/PFT/1/Q2apM?_a=ChgyMDIyMDUxMzEyMzUwMjMzMTo1MjAyODASBTg4MjU5GgpPTkVfU0VBUkNIIg4xNTguMTExLjIzNi45NSoGMTA1NzQ0MgoyNjYxNzQxNzE2Og1Eb2N1bWVudEltYWdlQgEwUgZPbmxpbmVaAkZUYgNQRlRqCjIwMjIvMDUvMDFyCjIwMjIvMDUvMTR6AIIBKVAtMTAwNzg1Mi0yNjcyNC1DVVNUT01FUi0xMDAwMDI1NS01NzY0MzExkgEGT25saW5lygFzTW96aWxsYS81LjAgKFdpbmRvd3MgTlQgMTAuMDsgV2luNjQ7IHg2NCkgQXBwbGVXZWJLaXQvNTM3LjM2IChLSFRNTCwgbGlrZSBHZWNrbykgQ2hyb21lLzEwMS4wLjQ5NTEuNjQgU2FmYXJpLzUzNy4zNtIBElNjaG9sYXJseSBKb3VybmFsc5oCB1ByZVBhaWSqAitPUzpFTVMtTWVkaWFMaW5rc1NlcnZpY2UtZ2V0TWVkaWFVcmxGb3JJdGVtygIPQXJ0aWNsZXxGZWF0dXJl0gIBWfICAPoCAVmCAwNXZWKKAxxDSUQ6MjAyMjA1MTMxMjM1MDIzMzE6OTE2ODk3&_s=4R%2BrSLBAOWkAv60BD6umfsLkEuQ%3D

Crop Residue Burning Emissions and the Impact on Ambient Particulate Matters over South Korea

In the study, crop residue burning (CRB) emissions were estimated based on field surveys and combustion experiments to assess the impact of the CRB on particulate matter over South Korea. The estimates of CRB emissions over South Korea are 9514, 8089, 4002, 2010, 172,407, 7675, 33, and 5053 Mg year−1 for PM10, PM2.5, OC, EC, CO, NOx, SO2, and NH3, respectively. Compared with another study, our estimates in the magnitudes of CRB emissions were not significantly different. When the CRB emissions are additionally considered in the simulation, the monthly mean differences in PM2.5 (i.e., △PM2.5) were marginal between 0.07 and 0.55 μg m−3 over South Korea. Those corresponded to 0.6–4.3% in relative differences. Additionally, the △PM10 was 0.07–0.60 μg m−3 over South Korea. In the spatial and temporal aspects, the increases in PM10 and PM2.5 were high in Gyeongbuk (GB) and Gyeongnam (GN) provinces in June, October, November, and December.

Insights into the significant increase in ozone during COVID-19 in a typical urban city of China

The outbreak of COVID-19 promoted strict restrictions to human activities in China, which led to a dramatic decrease in most air pollutant concentrations (e.g., PM2.5, PM10, NOx, SO2 and CO). However, an obvious increase in ozone (O3) concentrations was found during the lockdown period in most urban areas of China. In this study, we conducted field measurements targeting ozone and its key precursors by utilizing a novel proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) in Changzhou, which is representative of the Yangtze River Delta (YRD) city cluster of China. We further applied the integrated methodology including machine learning, an observation-based model (OBM) and sensitivity analysis to obtain insights into the reasons causing the obvious increase in ozone. Major findings include the following: (1) by deweathered calculation, we found changes in precursor emissions contributed 1.46 ppbv to the increase in the observed O3 during the full-lockdown period in 2020, while meteorology constrained 3.0 ppbv of O3 in the full-lockdown period of 2019. (2) By using an OBM, we found that although a significant reduction in O3 precursors was observed during the full-lockdown period, the photochemical formation of O3 was stronger than that during the pre-lockdown period. (3) The NOx/VOC ratio dropped dramatically from 1.84 during the pre-lockdown to 0.79 in the full-lockdown period, which switched O3 formation from a VOC-limited regime to the boundary of a NOx- and VOC-limited regime. Additionally, box model results suggested that the decrease in the NOx/VOC ratio during the full-lockdown period could increase the mean O3 by 2.4 ppbv. Results of this study give insights into the relationship between O3 and its precursors in urban area and demonstrate reasons for the obvious increase in O3 in most urban areas of China during the COVID-19 lockdown period. This study also underlines the necessity of controlling anthropogenic oxygenated volatile organic compounds (OVOCs), alkenes and aromatics in the sustained campaign of reducing O3 pollution in China.

Temporal variation analysis, impact of COVID-19 on air pollutant concentrations, and forecasting of air pollutants over the cities of Bangalore and Delhi in India

Indian cities are highly vulnerable to atmospheric pollution in recent years, due to exponential growth in urbanisation and industrialisation, and the increased pollution has been made to focus on the temporal variation analysis and forecasting of air pollutants over major Indian cities like Delhi and Bangalore. PM2.5 concentrations are nearly 60.5% less than the annual average value during monsoon season while 76.3% more during the winter months. Ozone concentrations increase during the summer months (~ 46.3% more than the annual average) in Delhi, whereas in Bangalore, ozone concentrations are more (~ 75% more than the annual average) during the winter months. Variations of carbon monoxide and nitrogen oxides are significantly less comparatively. COVID-19 lockdown has a substantial positive impact on air pollution. Air pollutant concentrations are reduced during phase I and phase II of the lockdown. Pollutants, especially NOx and PM2.5 concentrations, are drastically reduced compared to the previous years. NOx concentrations are reduced by ~ 20% in Bangalore, whereas ~ 50% in Delhi. PM2.5 concentrations are reduced by ~ 41% in Delhi and ~ 55% in Bangalore. Forecasting of pollutants will be helpful in providing the valuable information for the optimal air pollution control strategies. It has been observed that linear model gives better results compared to ARIMA and Exponential Smoothening models. By forecasting, the concentration of NO2 is 115.288 µg/m3, the ozone is 30.636 µg/m3, SO2 is 11.798 µg/m3, and CO is 2.758 mg/m3 over Delhi in 2021. All the pollutants during forecasting showed a rising trend except sulphur dioxide.

Ozone pollution during the COVID-19 lockdown in the spring of 2020 over Europe, analysed from satellite observations, in situ measurements, and models

We present a comprehensive study integrating satellite observations of ozone pollution, in situ measurements, and chemistry-transport model simulations for quantifying the role of anthropogenic emission reductions during the COVID-19 lockdown in spring 2020 over Europe. Satellite observations are derived from the IASI+GOME2 (Infrared Atmospheric Sounding Interferometer + Global Ozone Monitoring Experiment 2) multispectral synergism, which provides better sensitivity to near-surface ozone pollution. These observations are mainly analysed in terms of differences between the average on 1–15 April 2020, when the strictest lockdown restrictions took place, and the same period in 2019. They show clear enhancements of near-surface ozone in central Europe and northern Italy, as well as some other hotspots, which are typically characterized by volatile organic compound (VOC)-limited chemical regimes. An overall reduction of ozone is observed elsewhere, where ozone chemistry is limited by the abundance of NOx. The spatial distribution of positive and negative ozone concentration anomalies observed from space is in relatively good quantitative agreement with surface in situ measurements over the continent (a correlation coefficient of 0.55, a root-mean-squared difference of 11 ppb, and the same standard deviation and range of variability). An average difference of ∼ 8 ppb between the two observational datasets is observed, which can partly be explained by the fact the satellite approach retrieves partial columns of ozone with a peak sensitivity above the surface (near 2 km of altitude over land and averaging kernels reaching the middle troposphere over ocean).For assessing the impact of the reduction of anthropogenic emissions during the lockdown, we adjust the satellite and in situ surface observations for subtracting the influence of meteorological conditions in 2020 and 2019. This adjustment is derived from the chemistry-transport model simulations using the meteorological fields of each year and identical emission inventories. Using adjustments adapted for the altitude and sensitivity of each observation, both datasets show consistent estimates of the influence of lockdown emission reduction. They both show lockdown-associated ozone enhancements in hotspots over central Europe and northern Italy, with a reduced amplitude with respect to the total changes observed between the 2 years and an overall reduction elsewhere over Europe and the ocean. Satellite observations additionally provide the ozone anomalies in the regions remote from in situ sensors, an enhancement over the Mediterranean likely associated with maritime traffic emissions, and a marked large-scale reduction of ozone elsewhere over ocean (particularly over the North Sea), in consistency with previous assessments done with ozone sonde measurements in the free troposphere.These observational assessments are compared with model-only estimations, using the CHIMERE chemistry-transport model. Whereas a general qualitative consistency of positive and negative ozone anomalies is observed with respect to observational estimates, significant changes are seen in their amplitudes. Models underestimate the range of variability of the ozone changes by at least a factor 2 with respect to the two observational datasets, both for enhancements and decreases of ozone. Moreover, a significant ozone decrease observed at a large hemispheric scale is not simulated since the modelling domain is the European continent. As simulations only consider the troposphere, the influence from stratospheric ozone is also missing. Sensitivity analyses also show an important role of vertical mixing of atmospheric constituents, which depends on the meteorological fields used in the simulation and significantly modify the amplitude of the changes of ozone pollution during the lockdown.

High atmospheric oxidation capacity drives wintertime nitrate pollution in the eastern Yangtze River Delta of China

Nitrate aerosol plays an increasingly important role in wintertime haze pollution in China. Despite intensive research on wintertime nitrate chemistry in recent years, quantitative constraints on the formation mechanisms of nitrate aerosol in the Yangtze River Delta (YRD), one of the most developed and densely populated regions in eastern China, remain inadequate. In this study, we identify the major nitrate formation pathways and their key controlling factors during the winter haze pollution period in the eastern YRD using 2-year (2018–2019) field observations and detailed observation-constrained model simulations. We find that the high atmospheric oxidation capacity, coupled with high aerosol liquid water content (ALWC), made both the heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) and the gas-phase OH oxidation of nitrogen dioxide (NO2) important pathways for wintertime nitrate formation in this region, with contribution percentages of 69 % and 29 % in urban areas and 63 % and 35 % in suburban areas during the haze pollution episodes, respectively. We further find that the gas-to-particle partitioning of nitric acid (HNO3) was very efficient so that the rate-determining step in the overall formation process of nitrate aerosol was the oxidation of NOx to HNO3 through both heterogeneous and gas-phase processes. The atmospheric oxidation capacity (i.e., the availability of O3 and OH radicals) was the key factor controlling the production rate of HNO3 from both processes. During the COVID-19 lockdown (January–February 2020), the enhanced atmospheric oxidation capacity greatly promoted the oxidation of NOx to nitrate and hence weakened the response of nitrate aerosol to the emission reductions in urban areas. Our study sheds light on the detailed formation mechanisms of wintertime nitrate aerosol in the eastern YRD and highlights the demand for the synergetic regulation of atmospheric oxidation capacity and NOx emissions to mitigate wintertime nitrate and haze pollution in eastern China.