Changing Responses of PM2.5 and Ozone to Source Emissions in the Yangtze River Delta Using the Adjoint Model.

China's industrial restructuring and pollution controls have altered the contributions of individual sources to varying air quality over the past decade. We used the GEOS-Chem adjoint model and investigated the changing sensitivities of PM2.5 and ozone (O3) to multiple species and sources from 2010 to 2020 in the central Yangtze River Delta (YRDC), the largest economic region in China. Controlling primary particles and SO2 from industrial and residential sectors dominated PM2.5 decline, and reducing CO from multiple sources and ≥C3 alkenes from vehicles restrained O3. The chemical regime of O3 formation became less VOC-limited, attributable to continuous NOX abatement for specific sources, including power plants, industrial combustion, cement production, and off-road traffic. Regional transport was found to be increasingly influential on PM2.5. To further improve air quality, management of agricultural activities to reduce NH3 is essential for alleviating PM2.5 pollution, while controlling aromatics, alkenes, and alkanes from industry and gasoline vehicles is effective for O3. Reducing the level of NOX from nearby industrial combustion and transportation is helpful for both species. Our findings reveal the complexity of coordinating control of PM2.5 and O3 pollution in a fast-developing region and support science-based policymaking for other regions with similar air pollution problems.

Societal shifts due to COVID-19 reveal large-scale complexities and feedbacks between atmospheric chemistry and climate change.

The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheric composition. The resulting reductions in anthropogenic activity represent an unprecedented event that yields a glimpse into a future where emissions to the atmosphere are reduced. Furthermore, the abrupt reduction in emissions during the lockdown periods led to clearly observable changes in atmospheric composition, which provide direct insight into feedbacks between the Earth system and human activity. While air pollutants and greenhouse gases share many common anthropogenic sources, there is a sharp difference in the response of their atmospheric concentrations to COVID-19 emissions changes, due in large part to their different lifetimes. Here, we discuss several key takeaways from modeling and observational studies. First, despite dramatic declines in mobility and associated vehicular emissions, the atmospheric growth rates of greenhouse gases were not slowed, in part due to decreased ocean uptake of CO2 and a likely increase in CH4 lifetime from reduced NO x emissions. Second, the response of O3 to decreased NO x emissions showed significant spatial and temporal variability, due to differing chemical regimes around the world. Finally, the overall response of atmospheric composition to emissions changes is heavily modulated by factors including carbon-cycle feedbacks to CH4 and CO2, background pollutant levels, the timing and location of emissions changes, and climate feedbacks on air quality, such as wildfires and the ozone climate penalty.

Global Health and Climate Effects of Organic Aerosols from Different Sources.

The impact of aerosols on human health and climate is well-recognized, yet many studies have only focused on total PM2.5 or changes from anthropogenic activities. This study quantifies the health and climate effects of organic aerosols (OA) from anthropogenic, biomass burning, and biogenic sources. Using two atmospheric chemistry models, CAM-chem and GEOS-Chem, our findings reveal that anthropogenic primary OA (POA) has the highest efficiency for health effects but the lowest for direct radiative effects due to spatial and temporal variations associated with population and surface albedo. The treatment of POA as nonvolatile or semivolatile also influences these efficiencies through different chemical processes. Biogenic OA shows moderate efficiency for health effects and the highest for direct radiative effects but has the lowest efficiency for indirect effects due to the reduced high cloud, caused by stabilized temperature profiles from aerosol-radiation interactions in biogenic OA-rich regions. Biomass burning OA is important for cloud radiative effect changes in remote atmospheres due to its ability to be transported further than other OAs. This study highlights the importance of not only OA characteristics such as toxicity and refractive index but also atmospheric processes such as transport and chemistry in determining health and climate impact efficiencies.

Impacts and mitigation of excess diesel-related NOx emissions in 11 major vehicle markets.

Vehicle emissions contribute to fine particulate matter (PM2.5) and tropospheric ozone air pollution, affecting human health, crop yields and climate worldwide. On-road diesel vehicles produce approximately 20 per cent of global anthropogenic emissions of nitrogen oxides (NOx), which are key PM2.5 and ozone precursors. Regulated NOx emission limits in leading markets have been progressively tightened, but current diesel vehicles emit far more NOx under real-world operating conditions than during laboratory certification testing. Here we show that across 11 markets, representing approximately 80 per cent of global diesel vehicle sales, nearly one-third of on-road heavy-duty diesel vehicle emissions and over half of on-road light-duty diesel vehicle emissions are in excess of certification limits. These excess emissions (totalling 4.6 million tons) are associated with about 38,000 PM2.5- and ozone-related premature deaths globally in 2015, including about 10 per cent of all ozone-related premature deaths in the 28 European Union member states. Heavy-duty vehicles are the dominant contributor to excess diesel NOx emissions and associated health impacts in almost all regions. Adopting and enforcing next-generation standards (more stringent than Euro 6/VI) could nearly eliminate real-world diesel-related NOx emissions in these markets, avoiding approximately 174,000 global PM2.5- and ozone-related premature deaths in 2040. Most of these benefits can be achieved by implementing Euro VI standards where they have not yet been adopted for heavy-duty vehicles.

Air pollution mitigation assessment to inform Cambodia's first clean air plan.

Cambodia's 16.5 million people are exposed to air pollution in excess of World Health Organisation guidelines. The Royal Government of Cambodia has regulated air pollutant emissions and concentrations since 2000, but rapid economic growth and energy consumption means air pollution continues to impact human health. In December 2021, the Ministry of Environment of Cambodia published Cambodia's first Clean Air Plan that outlines actions to reduce air pollutant emissions over the next decade. This work presents the quantitative air pollution mitigation assessment underpinning the identification and evaluation of measures included in Cambodia's Clean Air Plan. Historic emissions of particulate matter (PM2.5, black carbon, organic carbon) and gaseous (nitrogen oxides, volatile organic compounds, sulphur dioxide, ammonia, and carbon monoxide) air pollutants are quantified between 2010 and 2015, and projected to 2030 for a baseline scenario. Mitigation scenarios reflecting implementation of 14 measures included in Cambodia's Clean Air Plan were modelled, to quantify the national reduction in emissions, from which the reduction in ambient PM2.5 exposure and attributable health burdens were estimated. In 2015, the residential, transport, and waste sectors contribute the largest fraction of national total air pollutant emissions. Without emission reduction measures, air pollutant emissions could increase by between 50 and 150% in 2030 compared to 2015 levels, predominantly due to increases in transport emissions. The implementation of the 14 mitigation measures could substantially reduce emissions of all air pollutants, by between 60 and 80% in 2030 compared to the baseline. This reduction in emissions was estimated to avoid approximately 900 (95% C.I.: 530-1200) premature deaths per year in 2030 compared to the baseline scenario. In addition to improving air pollution and public health, Cambodia's Clean Air Plan could also to lead to additional benefits, including a 19% reduction in carbon dioxide emissions, simultaneously contributing to Cambodia's climate change goals.

Sector-Based Top-Down Estimates of NO x , SO2, and CO Emissions in East Asia.

Top-down estimates using satellite data provide important information on the sources of air pollutants. We develop a sector-based 4D-Var framework based on the GEOS-Chem adjoint model to address the impacts of co-emissions and chemical interactions on top-down emission estimates. We apply OMI NO2, OMI SO2, and MOPITT CO observations to estimate NO x , SO2, and CO emissions in East Asia during 2005-2012. Posterior evaluations with surface measurements show reduced normalized mean bias (NMB) by 7% (NO2)-15% (SO2) and normalized mean square error (NMSE) by 8% (SO2)-9% (NO2) compared to a species-based inversion. This new inversion captures the peak years of Chinese SO2 (2007) and NO x (2011) emissions and attributes their drivers to industry and energy activities. The CO peak in 2007 in China is driven by residential and industry emissions. In India, the inversion attributes NO x and SO2 trends mostly to energy and CO trend to residential emissions.

Sources of ambient PM2.5 exposure in 96 global cities.

To improve air quality, knowledge of the sources and locations of air pollutant emissions is critical. However, for many global cities, no previous estimates exist of how much exposure to fine particulate matter (PM2.5), the largest environmental cause of mortality, is caused by emissions within the city vs. outside its boundaries. We use the Intervention Model for Air Pollution (InMAP) global-through-urban reduced complexity air quality model with a high-resolution, global inventory of pollutant emissions to quantify the contribution of emissions by source type and location for 96 global cities. Among these cities, we find that the fraction of PM2.5 exposure caused by within-city emissions varies widely (µ = 37%; σ = 22%) and is not well-explained by surrounding population density. The list of most-important sources also varies by city. Compared to a more mechanistically detailed model, InMAP predicts urban measured concentrations with lower bias and error but also lower correlation. Predictive accuracy in urban areas is not particularly high with either model, suggesting an opportunity for improving global urban air emission inventories. We expect the results herein can be useful as a screening tool for policy options and, in the absence of available resources for further analysis, to inform policy action to improve public health.

Sensitivities of Ozone Air Pollution in the Beijing-Tianjin-Hebei Area to Local and Upwind Precursor Emissions Using Adjoint Modeling.

Effective mitigation of surface ozone pollution entails detailed knowledge of the contributing precursors' sources. We use the GEOS-Chem adjoint model to analyze the precursors contributing to surface ozone in the Beijing-Tianjin-Hebei area (BTH) of China on days of different ozone pollution severities in June 2019. We find that BTH ozone on heavily polluted days is sensitive to local emissions, as well as to precursors emitted from the provinces south of BTH (Shandong, Henan, and Jiangsu, collectively the SHJ area). Heavy ozone pollution in BTH can be mitigated effectively by reducing NOx (from industrial processes and transportation), ≥C3 alkenes (from on-road gasoline vehicles and industrial processes), and xylenes (from paint use) emitted from both BTH and SHJ, as well as by reducing CO (from industrial processes, transportation, and power generation) and ≥C4 alkanes (from industrial processes, paint and solvent use, and on-road gasoline vehicles) emissions from SHJ. In addition, reduction of NOx, xylene, and ≥C3 alkene emissions within BTH would effectively decrease the number of BTH ozone-exceedance days. Our analysis pinpoint the key areas and activities for locally and regionally coordinated emission control efforts to improve surface ozone air quality in BTH.

Unexpected slowdown of US pollutant emission reduction in the past decade.

Ground and satellite observations show that air pollution regulations in the United States (US) have resulted in substantial reductions in emissions and corresponding improvements in air quality over the last several decades. However, large uncertainties remain in evaluating how recent regulations affect different emission sectors and pollutant trends. Here we show a significant slowdown in decreasing US emissions of nitrogen oxides (NO x ) and carbon monoxide (CO) for 2011-2015 using satellite and surface measurements. This observed slowdown in emission reductions is significantly different from the trend expected using US Environmental Protection Agency (EPA) bottom-up inventories and impedes compliance with local and federal agency air-quality goals. We find that the difference between observations and EPA's NO x emission estimates could be explained by: (i) growing relative contributions of industrial, area, and off-road sources, (ii) decreasing relative contributions of on-road gasoline, and (iii) slower than expected decreases in on-road diesel emissions.

Global Estimates and Long-Term Trends of Fine Particulate Matter Concentrations (1998-2018).

Exposure to outdoor fine particulate matter (PM2.5) is a leading risk factor for mortality. We develop global estimates of annual PM2.5 concentrations and trends for 1998-2018 using advances in satellite observations, chemical transport modeling, and ground-based monitoring. Aerosol optical depths (AODs) from advanced satellite products including finer resolution, increased global coverage, and improved long-term stability are combined and related to surface PM2.5 concentrations using geophysical relationships between surface PM2.5 and AOD simulated by the GEOS-Chem chemical transport model with updated algorithms. The resultant annual mean geophysical PM2.5 estimates are highly consistent with globally distributed ground monitors (R2 = 0.81; slope = 0.90). Geographically weighted regression is applied to the geophysical PM2.5 estimates to predict and account for the residual bias with PM2.5 monitors, yielding even higher cross validated agreement (R2 = 0.90-0.92; slope = 0.90-0.97) with ground monitors and improved agreement compared to all earlier global estimates. The consistent long-term satellite AOD and simulation enable trend assessment over a 21 year period, identifying significant trends for eastern North America (-0.28 ± 0.03 µg/m3/yr), Europe (-0.15 ± 0.03 µg/m3/yr), India (1.13 ± 0.15 µg/m3/yr), and globally (0.04 ± 0.02 µg/m3/yr). The positive trend (2.44 ± 0.44 µg/m3/yr) for India over 2005-2013 and the negative trend (-3.37 ± 0.38 µg/m3/yr) for China over 2011-2018 are remarkable, with implications for the health of billions of people.

Transient climate and ambient health impacts due to national solid fuel cookstove emissions.

Residential solid fuel use contributes to degraded indoor and ambient air quality and may affect global surface temperature. However, the potential for national-scale cookstove intervention programs to mitigate the latter issues is not yet well known, owing to the spatial heterogeneity of aerosol emissions and impacts, along with coemitted species. Here we use a combination of atmospheric modeling, remote sensing, and adjoint sensitivity analysis to individually evaluate consequences of a 20-y linear phase-out of cookstove emissions in each country with greater than 5% of the population using solid fuel for cooking. Emissions reductions in China, India, and Ethiopia contribute to the largest global surface temperature change in 2050 [combined impact of -37 mK (11 mK to -85 mK)], whereas interventions in countries less commonly targeted for cookstove mitigation such as Azerbaijan, Ukraine, and Kazakhstan have the largest per cookstove climate benefits. Abatement in China, India, and Bangladesh contributes to the largest reduction of premature deaths from ambient air pollution, preventing 198,000 (102,000-204,000) of the 260,000 (137,000-268,000) global annual avoided deaths in 2050, whereas again emissions in Ukraine and Azerbaijan have the largest per cookstove impacts, along with Romania. Global cookstove emissions abatement results in an average surface temperature cooling of -77 mK (20 mK to -278 mK) in 2050, which increases to -118 mK (-11 mK to -335 mK) by 2100 due to delayed CO2 response. Health impacts owing to changes in ambient particulate matter with an aerodynamic diameter of 2.5 µm or less (PM2.5) amount to ∼22.5 million premature deaths prevented between 2000 and 2100.

Improving present day and future estimates of anthropogenic sectoral emissions and the resulting air quality impacts in Africa.

The African continent is undergoing immense social and economic change, particularly regarding population growth and urbanization, where the urban population in Africa is anticipated to increase by a factor of 3 over the next 40 years. To understand the potential health impacts from this demographical shift and design efficient emission mitigation strategies, we used improved Africa-specific emissions that account for inefficient combustion sources for a number of sectors such as transportation, household energy generation, waste burning, and home heating and cooking. When these underrepresented emissions sources are combined with the current estimates of emissions in Africa, ambient particulate matter concentrations from present-day anthropogenic activity contribute to 13 210 annual premature deaths, with the largest contributions (38%) coming from residential emissions. By scaling both the population and the emissions for projected national-scale levels of growth, the predicted health impact grows to approximately 78 986 annual premature deaths by 2030 with 45% now resulting from emissions related to energy combustion. In order to mitigate this resulting increase in premature deaths, three scenarios have been developed which reduce sector-specific future emissions based on prior targets for technological improvements and emission controls in transportation, energy production and residential activities. These targeted potential mitigation strategies can avoid up to 37% of the estimated annual premature deaths by 2030 with the largest opportunity being a reduction of 10 868 annual deaths from switching half of the energy generation in South Africa to renewable technologies.

Emission Impacts of Electric Vehicles in the US Transportation Sector Following Optimistic Cost and Efficiency Projections.

This study investigates emission impacts of introducing inexpensive and efficient electric vehicles into the US light duty vehicle (LDV) sector. Scenarios are explored using the ANSWER-MARKAL model with a modified version of the Environmental Protection Agency's (EPA) 9-region database. Modified cost and performance projections for LDV technologies are adapted from the National Research Council (2013) optimistic case. Under our optimistic scenario (OPT) we find 15% and 47% adoption of battery electric vehicles (BEVs) in 2030 and 2050, respectively. In contrast, gasoline vehicles (ICEVs) remain dominant through 2050 in the EPA reference case (BAU). Compared to BAU, OPT gives 16% and 36% reductions in LDV greenhouse gas (GHG) emissions for 2030 and 2050, respectively, corresponding to 5% and 9% reductions in economy-wide emissions. Total nitrogen oxides, volatile organic compounds, and SO2 emissions are similar in the two scenarios due to intersectoral shifts. Moderate, economy-wide GHG fees have little effect on GHG emissions from the LDV sector but are more effective in the electricity sector. In the OPT scenario, estimated well-to-wheels GHG emissions from full-size BEVs with 100-mile range are 62 gCO2-e mi-1 in 2050, while those from full-size ICEVs are 121 gCO2-e mi-1.

Impacts of Foreign, Domestic, and State-Level Emissions on Ozone-Induced Vegetation Loss in the United States.

Exposure to elevated levels of ozone leads to yield reduction in agricultural crops and biomass loss in trees. Here, we quantify the impact of ozone pollution on two major U.S. crops, wheat and soybean, and two ozone-sensitive tree species, ponderosa pine and quaking aspen, using simulations with the GEOS-Chem model for 2010. Using previously established exposure-response functions, we estimate nationwide relative yield reductions of 4.9% for wheat and 6.7% for soybean, and relative biomass loss of 2.5% and 2.9% for ponderosa pine and aspen seedlings, respectively. Adjoint model sensitivities are used to estimate the impact of emissions sources from different locations, species, and sectors. We find that the nationwide relative loss in each vegetation type is influenced most by domestic anthropogenic NOx (>75%). Long-range transport from foreign sources is small relative to domestic influences. More than half of the anthropogenic NOx responsible for vegetation damage originates from outside the states where the damage occurs. Texas and Missouri are the highest contributors to the nationwide loss of wheat and soybean, respectively. California "exports" ozone damage for all types of vegetation studied, due to its location, high share of anthropogenic NOx, and a relatively low share of vegetation.

Sources and Processes Affecting Fine Particulate Matter Pollution over North China: An Adjoint Analysis of the Beijing APEC Period.

The stringent emission controls during the APEC 2014 (the Asia-Pacific Economic Cooperation Summit; November 5-11, 2014) offer a unique opportunity to quantify factors affecting fine particulate matter (PM2.5) pollution over North China. Here we apply a four-dimensional variational data assimilation system using the adjoint model of GEOS-Chem to address this issue. Hourly surface measurements of PM2.5 and SO2 for October 15-November 14, 2014 are assimilated into the model to optimize daily aerosol primary and precursor emissions over North China. Measured PM2.5 concentrations in Beijing average 50.3 µg m(-3) during APEC, 43% lower than the mean concentration (88.2 µg m(-3)) for the whole period including APEC. Model results attribute about half of the reduction to meteorology due to active cold surge occurrences during APEC. Assimilation of surface measurements largely reduces the model biases and estimates 6%-30% lower aerosol emissions in the Beijing-Tianjin-Hebei region during APEC than in late October. We further demonstrate that high PM2.5 events in Beijing during this period can be occasionally contributed by natural mineral dust, but more events show large sensitivities to inorganic aerosol sources, particularly emissions of ammonia (NH3) and nitrogen oxides (NOx) reflecting strong formation of aerosol nitrate in the fall season.

Response of global particulate-matter-related mortality to changes in local precursor emissions.

Recent Global Burden of Disease (GBD) assessments estimated that outdoor fine-particulate matter (PM2.5) is a causal factor in over 5% of global premature deaths. PM2.5 is produced by a variety of direct and indirect, natural and anthropogenic processes that complicate PM2.5 management. This study develops a proof-of-concept method to quantify the effects on global premature mortality of changes to PM2.5 precursor emissions. Using the adjoint of the GEOS-Chem chemical transport model, we calculated sensitivities of global PM2.5-related premature mortality to emissions of precursor gases (SO2, NOx, NH3) and carbonaceous aerosols. We used a satellite-derived ground-level PM2.5 data set at approximately 10 × 10 km(2) resolution to better align the exposure with population density. We used exposure-response functions from the GBD project to relate mortality to exposure in the adjoint calculation. The response of global mortality to changes in local anthropogenic emissions varied spatially by several orders of magnitude. The largest reductions in mortality for a 1 kg km(-2) yr(-1) decrease in emissions were for ammonia and carbonaceous aerosols in Eastern Europe. The greatest reductions in mortality for a 10% decrease in emissions were found for secondary inorganic sources in East Asia. In general, a 10% decrease in SO2 emissions was the most effective source to control, but regional exceptions were found.

Differences between magnitudes and health impacts of BC emissions across the United States using 12 km scale seasonal source apportionment.

Recent assessments have analyzed the health impacts of PM2.5 from emissions from different locations and sectors using simplified or reduced-form air quality models. Here we present an alternative approach using the adjoint of the Community Multiscale Air Quality (CMAQ) model, which provides source-receptor relationships at highly resolved sectoral, spatial, and temporal scales. While damage resulting from anthropogenic emissions of BC is strongly correlated with population and premature death, we found little correlation between damage and emission magnitude, suggesting that controls on the largest emissions may not be the most efficient means of reducing damage resulting from anthropogenic BC emissions. Rather, the best proxy for locations with damaging BC emissions is locations where premature deaths occur. Onroad diesel and nonroad vehicle emissions are the largest contributors to premature deaths attributed to exposure to BC, while onroad gasoline emissions cause the highest deaths per amount emitted. Emissions in fall and winter contribute to more premature deaths (and more per amount emitted) than emissions in spring and summer. Overall, these results show the value of the high-resolution source attribution for determining the locations, seasons, and sectors for which BC emission controls have the most effective health benefits.

Formation of Low Volatility Organic Compounds and Secondary Organic Aerosol from Isoprene Hydroxyhydroperoxide Low-NO Oxidation.

Gas-phase low volatility organic compounds (LVOC), produced from oxidation of isoprene 4-hydroxy-3-hydroperoxide (4,3-ISOPOOH) under low-NO conditions, were observed during the FIXCIT chamber study. Decreases in LVOC directly correspond to appearance and growth in secondary organic aerosol (SOA) of consistent elemental composition, indicating that LVOC condense (at OA below 1 µg m(-3)). This represents the first simultaneous measurement of condensing low volatility species from isoprene oxidation in both the gas and particle phases. The SOA formation in this study is separate from previously described isoprene epoxydiol (IEPOX) uptake. Assigning all condensing LVOC signals to 4,3-ISOPOOH oxidation in the chamber study implies a wall-loss corrected non-IEPOX SOA mass yield of ∼4%. By contrast to monoterpene oxidation, in which extremely low volatility VOC (ELVOC) constitute the organic aerosol, in the isoprene system LVOC with saturation concentrations from 10(-2) to 10 µg m(-3) are the main constituents. These LVOC may be important for the growth of nanoparticles in environments with low OA concentrations. LVOC observed in the chamber were also observed in the atmosphere during SOAS-2013 in the Southeastern United States, with the expected diurnal cycle. This previously uncharacterized aerosol formation pathway could account for ∼5.0 Tg yr(-1) of SOA production, or 3.3% of global SOA.

Atmospheric reduced nitrogen: Sources, transformations, effects, and management.

Human activities have increased atmospheric emissions and deposition of oxidized and reduced forms of nitrogen, but emission control programs have largely focused on oxidized nitrogen. As a result, in many regions of the world emissions of oxidized nitrogen are decreasing while emissions of reduced nitrogen are increasing. Emissions of reduced nitrogen largely originate from livestock waste and fertilizer application, with contributions from transportation sources in urban areas. Observations suggest a discrepancy between trends in emissions and deposition of reduced nitrogen in the U.S., likely due to an underestimate in emissions. In the atmosphere, ammonia reacts with oxides of sulfur and nitrogen to form fine particulate matter that impairs health and visibility and affects climate forcings. Recent reductions in emissions of sulfur and nitrogen oxides have limited partitioning with ammonia, decreasing long-range transport. Continuing research is needed to improve understanding of how shifting emissions alter formation of secondary particulates and patterns of transport and deposition of reactive nitrogen. Satellite remote sensing has potential for monitoring atmospheric concentrations and emissions of ammonia, but there remains a need to maintain and strengthen ground-based measurements and continue development of chemical transport models. Elevated nitrogen deposition has decreased plant and soil microbial biodiversity and altered the biogeochemical function of terrestrial, freshwater, and coastal ecosystems. Further study is needed on differential effects of oxidized versus reduced nitrogen and pathways and timescales of ecosystem recovery from elevated nitrogen deposition. Decreases in deposition of reduced nitrogen could alleviate exceedances of critical loads for terrestrial and freshwater indicators in many U.S. areas. The U.S. Environmental Protection Agency should consider using critical loads as a basis for setting standards to protect public welfare and ecosystems. The U.S. and other countries might look to European experience for approaches to control emissions of reduced nitrogen from agricultural and transportation sectors.Implications: In this Critical Review we synthesize research on effects, air emissions, environmental transformations, and management of reduced forms of nitrogen. Emissions of reduced nitrogen affect human health, the structure and function of ecosystems, and climatic forcings. While emissions of oxidized forms of nitrogen are regulated in the U.S., controls on reduced forms are largely absent. Decreases in emissions of sulfur and nitrogen oxides coupled with increases in ammonia are shifting the gas-particle partitioning of ammonia and decreasing long-range atmospheric transport of reduced nitrogen. Effort is needed to understand, monitor, and manage emissions of reduced nitrogen in a changing environment.

Sensitivities of ozone to its precursors during heavy ozone pollution events in the Yangtze River Delta using the adjoint method.

Although the concentrations of five basic ambient air pollutants in the Yangtze River Delta (YRD) have been reduced since the implementation of the "Air Pollution Prevention and Control Action Plan" in 2013, the ozone concentrations still increase. In order to explore the causes of ozone pollution in YRD, we use the GEOS-Chem and its adjoint model to study the sensitivities of ozone to its precursor emissions from different source regions and emission sectors during heavy ozone pollution events under typical circulation patterns. The Multi-resolution Emission Inventory for China (MEIC) of Tsinghua University and 0.25° × 0.3125° nested grids are adopted in the model. By using the T-mode principal component analysis (T-PCA), the circulation patterns of heavy ozone pollution days (observed MDA8 O3 concentrations ≥160 µg m-3) in Nanjing located in the center area of YRD from 2013 to 2019 are divided into four types, with the main features of Siberian Low, Lake Balkhash High, Northeast China Low, Yellow Sea High, and southeast wind at the surface. The adjoint results show that the contributions of emissions emitted from Jiangsu and Zhejiang are the largest to heavy ozone pollution in Nanjing. The 10 % reduction of anthropogenic NOx and NMVOCs emissions in Jiangsu, Zhejiang and Shanghai could reduce the ozone concentrations in Nanjing by up to 3.40 µg m-3 and 0.96 µg m-3, respectively. However, the reduction of local NMVOCs emissions has little effect on ozone concentrations in Nanjing, and the reduction of local NOx emissions would even increase ozone pollution. For different emissions sectors, industry emissions account for 31 %-74 % of ozone pollution in Nanjing, followed by transportation emissions (18 %-49 %). This study could provide the scientific basis for forecasting ozone pollution events and formulating accurate strategies of emission reduction.