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.

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.

Aviation contrail climate effects in the North Atlantic from 2016 to 2021

Around 5 % of anthropogenic radiative forcing (RF) is attributed to aviation CO2 and non-CO2 impacts. This paper quantifies aviation emissions and contrail climate forcing in the North Atlantic, one of the world's busiest air traffic corridors, over 5 years. Between 2016 and 2019, growth in CO2 (+3.13% yr-1) and nitrogen oxide emissions (+4.5 % yr-1) outpaced increases in flight distance (+3.05 % yr-1). Over the same period, the annual mean contrail cirrus net RF (204–280 mW m-2) showed significant inter-annual variability caused by variations in meteorology. Responses to COVID-19 caused significant reductions in flight distance travelled (-66%), CO2 emissions (-71%) and the contrail net RF (-66%) compared with the prior 1-year period. Around 12 % of all flights in this region cause 80 % of the annual contrail energy forcing, and the factors associated with strongly warming/cooling contrails include seasonal changes in meteorology and radiation, time of day, background cloud fields, and engine-specific non-volatile particulate matter (nvPM) emissions. Strongly warming contrails in this region are generally formed in wintertime, close to the tropopause, between 15:00 and 04:00 UTC, and above low-level clouds. The most strongly cooling contrails occur in the spring, in the upper troposphere, between 06:00 and 15:00 UTC, and without lower-level clouds. Uncertainty in the contrail cirrus net RF (216–238 mW m-2) arising from meteorology in 2019 is smaller than the inter-annual variability. The contrail RF estimates are most sensitive to the humidity fields, followed by nvPM emissions and aircraft mass assumptions. This longitudinal evaluation of aviation contrail impacts contributes a quantified understanding of inter-annual variability and informs strategies for contrail mitigation.

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.

Improved monitoring of shipping NO2 with TROPOMI: decreasing NOx emissions in European seas during the COVID-19 pandemic

TROPOMI (TROPOspheric Monitoring Instrument) measurements of tropospheric NO2 columns provide powerful information on emissions of air pollution by ships on open sea. This information is potentially useful for authorities to help determine the (non-)compliance of ships with increasingly stringent NOx emission regulations. We find that the information quality is improved further by recent upgrades in the TROPOMI cloud retrieval and an optimal data selection. We show that the superior spatial resolution of TROPOMI allows for the detection of several lanes of NO2 pollution ranging from the Aegean Sea near Greece to the Skagerrak in Scandinavia, which have not been detected with other satellite instruments before. Additionally, we demonstrate that under conditions of sun glint TROPOMI's vertical sensitivity to NO2 in the marine boundary layer increases by up to 60 %. The benefits of sun glint are most prominent under clear-sky situations when sea surface winds are low but slightly above zero (±2 m s-1). Beyond spatial resolution and sun glint, we examine for the first time the impact of the recently improved cloud algorithm on the TROPOMI NO2 retrieval quality, both over sea and over land. We find that the new FRESCO+ (Fast Retrieval Scheme for Clouds from the Oxygen A band) wide algorithm leads to 50 hPa lower cloud pressures, correcting a known high bias, and produces 1–4×1015 molec. cm-2 higher retrieved NO2 columns, thereby at least partially correcting for the previously reported low bias in the TROPOMI NO2 product. By training an artificial neural network on the four available periods with standard and FRESCO+ wide test retrievals, we develop a historic, consistent TROPOMI NO2 data set spanning the years 2019 and 2020. This improved data set shows stronger (35 %–75 %) and sharper (10 %–35 %) shipping NO2 signals compared to co-sampled measurements from OMI. We apply our improved data set to investigate the impact of the COVID-19 pandemic on ship NO2 pollution over European seas and find indications that NOx emissions from ships reduced by 10 %–20 % during the beginning of the COVID-19 pandemic in 2020. The reductions in ship NO2 pollution start in March–April 2020, in line with changes in shipping activity inferred from automatic identification system (AIS) data on ship location, speed, and engine.

Variability of nitrogen oxide emission fluxes and lifetimes estimated from Sentinel-5P TROPOMI observations

Satellite observations of the high-resolution TROPOspheric Monitoring Instrument (TROPOMI) on Sentinel-5 Precursor can be used to observe nitrogen dioxide (NO2) at city scales to quantify short time variability of nitrogen oxide (NOx) emissions and lifetimes on a daily and seasonal basis. In this study, 2 years of TROPOMI tropospheric NO2 columns, having a spatial resolution of up to 3.5 km × 5.5 km, have been analyzed together with wind and ozone data. NOx lifetimes and emission fluxes are estimated for 50 different NOx sources comprising cities, isolated power plants, industrial regions, oil fields, and regions with a mix of sources distributed around the world. The retrieved NOx emissions are in agreement with other TROPOMI-based estimates and reproduce the variability seen in power plant stack measurements but are in general lower than the analyzed stack measurements and emission inventory results. Separation into seasons shows a clear seasonal dependence of NOx emissions with in general the highest emissions during winter, except for isolated power plants and especially sources in hot desert climates, where the opposite is found. The NOx lifetime shows a systematic latitudinal dependence with an increase in lifetime from 2 to 8 h with latitude but only a weak seasonal dependence. For most of the 50 sources including the city of Wuhan in China, a clear weekly pattern of NOx emissions is found, with weekend-to-weekday ratios of up to 0.5 but with a high variability for the different locations. During the Covid-19 lockdown period in 2020, strong reductions in the NOx emissions were observed for New Delhi, Buenos Aires, and Madrid.

Measurement report: Fast photochemical production of peroxyacetyl nitrate (PAN) over the rural North China Plain during haze events in autumn

Photochemical pollution over the North China Plain (NCP) is attracting much concern. We usually view peroxyacetyl nitrate (PAN) as the second most important photochemical pollutant featuring high mixing ratios during warm seasons. Our observations at a background site in the NCP identified high PAN concentrations, even during haze events in autumn. The substantial increasing ratios of PAN, by 244 % and 178 %, over the morning hours (08:00–12:00 local time) on 20 and 25 October 2020 were 10.6 and 7.7 times larger than those on clean days. Polluted days are characterized by higher temperature, higher humidity, and anomalous southerly winds compared with clean days. Enhanced local photochemistry has been identified as being the dominant factor that controls the PAN increase in the morning at the rural site, as the time when prevailing wind turns to a southerly wind is too late to promote direct transport of PAN from the polluted urban region. By removing the effect of direct transport of PAN, we provide a quantitative assessment of net PAN chemical production rate of 0.45 ppb h-1 for the mornings of polluted days, also demonstrating the strong local photochemistry. Using observations and calculated photolysis rates, we find that acetaldehyde oxidation by hydroxyl radical (OH) is the primary pathway of peroxyacetyl radical formation at the rural site. Acetaldehyde concentrations and production rates of HOx (HOx= OH + HO2) on polluted days are 2.8 and 2 times as large as those on clean days, leading to a remarkable increase in PAN in the morning. Formaldehyde (HCHO) photolysis dominates the daytime HOx production, thus contributing to fast photochemistry of PAN. Our observational results suggest the cause of a rapid increase in PAN during haze events in autumn at a rural site of the NCP and provide evidence of important role of HCHO photolysis in secondary pollutants at lower nitrogen oxide emissions. This highlights the urgency of carrying out strict volatile organic compound controls over the NCP during the cold season and not just in summer.