Surface ozone (O 3 ) air pollution in populated regions has been attributed to emissions of nitrogen oxides (NO + NO 2 = NO x ) and reactive volatile organic compounds (VOCs). These constituents react with hydrogen oxide radicals (OH + HO 2 = HO x ) in the presence of sunlight and heat to produce O 3 . The question of whether to reduce NO x emissions, VOC emissions, or both is complicated by spatially and temporally heterogeneous ozone-NO x -VOC sensitivity. This study characterizes spatial and temporal variations in O 3 sensitivity by analyzing the ratio of formaldehyde (HCHO, a marker of VOCs) to nitrogen dioxide (NO 2 ), a metric known as the formaldehyde nitrogen ratio (FNR). Level 3 gridded retrievals from the Ozone Monitoring Instrument (OMI) aboard the NASA Aura satellite were used to calculate FNR, with our analysis focusing on China. Based on previous studies, we take FNR < 1.0 as indicating VOC-limited regimes, FNR > 2.0 as indicating NO x -limited regime, and FNR between 1.0 and 2.0 as indicating transitional regime (where either NO x reductions or VOC reductions would be expected to reduce O 3 ). We find that the transitional regime is widespread over the North China Plain (NCP), the Yangtze River Delta, and the Pearl River Delta during the ozone season (defined as having near-surface air temperatures >20°C at the early afternoon OMI overpass time). Outside of these regions, the NO x -limited regime is dominant. Because HCHO and NO 2 have distinct seasonal patterns, FNR also has a pronounced seasonality, consistent with the seasonal cycle of surface O 3 . Examining trends from 2005 to 2013 indicates rapid growth in NO 2 , especially over less-developed areas where O 3 photochemistry is NO x limited. Over this time period, HCHO decreased in southern China, where VOC emissions are dominated by biogenic sources, but increased slightly over the NCP, where VOC emissions are dominated by anthropogenic sources. A linear regression approach suggests that most of China (70% of grid cells) will be characterized by a transitional regime during the O 3 season by 2030. However, in megacities such as Guangzhou, Shanghai, and Beijing, NO 2 has decreased such that the chemical regime has shifted from VOC limited in 2005 to transitional in 2013.
Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NOx, and VOCs. The space‐based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identify NOx‐limited versus NOx‐saturated O3 formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NOx‐limited and NOx‐saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near‐surface environment, and (3) satellite products contain errors. We use the GEOS‐Chem global chemical transport model to evaluate the quantitative utility of FNR observed from the Ozone Monitoring Instrument over three northern midlatitude source regions. We find that FNR in the model surface layer is a robust predictor of the simulated near‐surface O3 production regime. Extending this surface‐based predictor to a column‐based FNR requires accounting for differences in the HCHO and NO2 vertical profiles. We compare four combinations of two OMI HCHO and NO2 retrievals with modeled FNR. The spatial and temporal correlations between the modeled and satellite‐derived FNR vary with the choice of NO2 product, while the mean offset depends on the choice of HCHO product. Space‐based FNR indicates that the spring transition to NOx‐limited regimes has shifted at least a month earlier over major cities (e.g., New York, London, and Seoul) between 2005 and 2015. This increase in NOx sensitivity implies that NOx emission controls will improve O3 air quality more now than it would have a decade ago.
Urban ozone (O3) formation can be limited by NO x , VOCs, or both, complicating the design of effective O3 abatement plans. A satellite-retrieved ratio of formaldehyde to NO2 (HCHO/NO2), developed from theory and modeling, has previously been used to indicate O3 formation chemistry. Here, we connect this space-based indicator to spatiotemporal variations in O3 recorded by on-the-ground monitors over major U.S. cities. High-O3 events vary nonlinearly with OMI HCHO and NO2, and the transition from VOC-limited to NO x -limited O3 formation regimes occurs at higher HCHO/NO2 value (3 to 4) than previously determined from models, with slight intercity variations. To extend satellite records back to 1996, we develop an approach to harmonize observations from GOME and SCIAMACHY that accounts for differences in spatial resolution and overpass time. Two-decade (1996–2016) multisatellite HCHO/NO2 captures the timing and location of the transition from VOC-limited to NO x -limited O3 production regimes in major U.S. cities, which aligns with the observed long-term changes in urban–rural gradient of O3 and the reversal of O3 weekend effect. Our findings suggest promise for applying space-based HCHO/NO2 to interpret local O3 chemistry, particularly with the new-generation satellite instruments that offer finer spatial and temporal resolution.
| Restrictions to reduce human interaction have helped to avoid greater suffering and death from the COVID-19 pandemic, but have also created socioeconomic hardship. This disruption is unprecedented in the modern era of global observing networks, pervasive sensing and large-scale tracking of human mobility and behaviour, creating a unique test bed for understanding the Earth System. In this Perspective, we hypothesize the immediate and long-term Earth System responses to COVID-19 along two multidisciplinary cascades: energy, emissions, climate and air quality; and poverty, globalization, food and biodiversity. While short-term impacts are dominated by direct effects arising from reduced human activity, longer-lasting impacts are likely to result from cascading effects of the economic recession on global poverty, green investment and human behaviour. These impacts offer the opportunity for novel insight, particularly with the careful deployment of targeted data collection, coordinated model experiments and solution-oriented randomized controlled trials, during and after the pandemic.
Fine particulate matter (PM 2.5 ) is a well-established risk factor for public health. To support both health risk assessment and epidemiological studies, data are needed on spatial and temporal patterns of PM 2.5 exposures. This review article surveys publicly available exposure datasets for surface PM 2.5 mass concentrations over the contiguous U.S., summarizes their applications and limitations, and provides suggestions on future research needs. The complex landscape of satellite instruments, model capabilities, monitor networks, and data synthesis methods offers opportunities for research development, but would benefit from guidance for new users. Guidance is provided to access publicly available PM 2.5 datasets, to explain and compare different approaches for dataset generation, and to identify sources of uncertainties associated with various types of datasets. Three main sources used to create PM 2.5 exposure data are: ground-based measurements (especially regulatory monitoring), satellite retrievals (especially aerosol optical depth, AOD), and atmospheric chemistry models. We find inconsistencies among several publicly available PM 2.5 estimates, highlighting uncertainties in the exposure datasets that are often overlooked in health effects analyses. Major differences among PM 2.5 estimates emerge from the choice of data (ground-based, satellite, and/or model), the spatiotemporal resolutions, and the algorithms used to fuse data sources.
Estimates of air pollution mortality in sub-Saharan Africa are limited by a lack of surface observations of fine particulate matter (PM2.5). Despite being large metropolises, Kinshasa, Democratic Republic of the Congo (DRC), population 14.3 million, and Brazzaville, Republic of the Congo (ROC),
Abstract. Biomass burning emits an estimated 25 % of global annual nitrogen oxides (NOx), an important constituent that participates in the oxidative chemistry of the atmosphere. Estimates of NOx emission factors, representing the amount of NOx per mass burned, are primarily based on field or laboratory case studies, but the sporadic and transient nature of wildfires makes it challenging to verify whether these case studies represent the behavior of the global fires that occur on earth. Satellite remote sensing provides a unique view of the earth, allowing for the study of emissions and downwind evolution of NOx from a large number of fires. We describe direct estimates of NOx emissions and lifetimes for fires using an exponentially modified Gaussian analysis of daily TROPOspheric Monitoring Instrument (TROPOMI) retrievals of NO2 tropospheric columns. We update the a priori profile of NO2 with a fine-resolution (0.25∘) global model simulation from NASA's GEOS Composition Forecasting System (GEOS-CF), which largely enhances NO2 columns over fire plumes. We derive representative NOx emission factors for six fuel types globally by linking TROPOMI-derived NOx emissions with observations of fire radiative power from Moderate Resolution Imaging Spectroradiometer (MODIS). Satellite-derived NOx emission factors are largely consistent with those derived from in situ measurements. We observe decreasing NOx lifetime with fire emissions, which we infer is due to the increase in both NOx abundance and hydroxyl radical production. Our findings suggest promise for applying space-based observations to track the emissions and chemical evolution of reactive nitrogen from wildfires.
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