Anthropogenic NOx Research Articles

Nontarget screening of a Siberian ice core reveals changes in the pre-industrial to industrial organic aerosol composition.

Glaciers serve as natural archives for reconstructing past changes of atmospheric aerosol concentration and composition. While most ice-core studies have focused on inorganic species, organic compounds, which can constitute up to 90% of the submicrometer aerosol mass, have been largely overlooked. To our knowledge, this study presents the first nontarget screening record of secondary organic aerosol species preserved in a Belukha ice core (Siberia, Russian Federation), ranging from the pre-industrial to the industrial period (1800-1980 CE). We identified a total of 398 molecules, primarily polar and low-volatile compounds. Since the 1950s, the atmospheric aerosol composition has changed, with the appearance of organic molecules, including nitrogen-containing compounds, deriving from enhanced atmospheric reactions with anthropogenic NOx, or direct emissions. In addition, there was a significant increase in the oxygen-to-carbon ratio (+3%) and the average carbon oxidation state (+18%) of the detected molecules compared to the pre-industrial period, suggesting an increased oxidative capacity of the atmosphere.

Summer urban synergistic effects of anthropogenic pollutants and low-molecular-weight biogenic volatile organic compounds on secondary organic aerosol presented by PM1.

Biogenic volatile organic compounds (BVOCs) are emitted by urban vegetation and can interact with anthropogenic pollutants to generate secondary organic aerosols (SOA) that are atmospheric pollutants in urban environments. In urban forests, SOA comprise up to 90% of all fine aerosols (particulate matter smaller than 1μm [PM1]) in the summer. PM1 can greatly affect urban air quality and public health. The formation of SOA is affected by both environmental conditions and the presence of light BVOCs-predominantly isoprene, pentene, butene, and 1,3-butadiene. These factors exhibit complex interactions and nonlinear relationships. In this study, high-frequency field observations were conducted in two urban forest sites in Shanghai during the summers of 2022 and 2023. Data were collected regarding the concentrations of light BVOCs; SOA; and the anthropogenic pollutants NOx, O3, and SO2, as well as solar radiation, temperature, and humidity. A model was developed to identify the synergistic effects of anthropogenic pollutants, meteorological factors, and BVOCs on SOA concentrations. Increases in short-term SOA concentrations were most strongly correlated with O3, which had a synergistic effect alongside NOx. The empirical analysis indicated that 0.144-0.585μg/m3 SOA is produced per μg/m3 of urban BVOCs but can be augmented by 0.072-0.491μg/m3 in the presence of O3, NOx, and SO2. However, long-term feedback mechanisms in urban forests contribute to the maintenance of stable SOA concentrations. The field data and models in this study provide a scientific basis for regulating atmospheric pollutants in urban forests under real-world conditions and offer intuitive and straightforward solutions for managing complex urban air pollution. Synopsis: Anthropogenic pollutants NOx, O3, and SO2 boost BVOCs' SOA production in summer urban forests. Short-term, pollutants are restrictive factors in SOA generation, but long-term forest SOA production exhibits negative feedback.

Spatiotemporal estimates of anthropogenic NOx emissions across China during 2015-2022 using a deep learning model.

As one of the significant air pollutants, nitrogen oxides (NOx = NO + NO2) not only pose a great threat to human health, but also contribute to the formation of secondary pollutants such as ozone and nitrate particles. Due to substantial uncertainties in bottom-up emission inventories, simulated concentrations of air pollutants using GEOS-Chem model often largely biased from those of ground-level observations. To address this issue, we developed a new deep learning model to simulate the inverse process of the GEOS-Chem model. This framework was applied to improve the total anthropogenic NOx emission intensity over a five-year period (2015-2019), and then to predict anthropogenic NOx emission intensity for 2020-2022. The deep learning model showed higher R2 value (0.94) based on 10-fold cross-validation, indicating that the model effectively captured spatial features and patterns. Then, NOx emission intensity was calibrated based on the new framework using high-resolution NO2 concentration dataset instead of the simulated NO2 levels derived from GEOS-Chem model. Overall, the top-down inversion result was in agreement with the bottom-up emission inventory at the spatial scale. The top-down emission fluxes were lower in high-emission regions such as central China, Beijing, Shanghai, the Pearl River Delta, and the central part of Liaoning, while posterior estimates were higher in regions with lower prior emission intensity. The posterior NOx emission intensity suggested that some major regions such as Beijing-Tianjin-Hebei (BTH) (-56.4 %) and Pearl River Delta (PRD) (-52.5 %) experienced dramatic NOx emission intensity decreases from 2015 to 2022, whereas some remote regions such as Tibetan Plateau remained relatively stable. This research contributes to the timely tracking of changes in pollutant emission and aids in the formulation of more effective and relevant pollution prevention and control policies.

Variation of biogenic VOC contribution to ozone formation with reduced anthropogenic precursor emissions: Coupling online observation and future scenario simulation.

As an essential component of urban natural sources, isoprene has strong interactions and synergies with anthropogenic precursors (volatile organic compounds and nitrogen oxides) of ozone (O3), influencing O3 formation in urban areas. However, the variability of these effects under different anthropogenic emission scenarios has not been fully understood. This study, utilizing observational data from Dezhou (a medium-sized city in the center of North China Plain) from May to September in both 2019 and 2020, and incorporating four future scenarios based on Shared Socioeconomic Pathways (SSP1-2.6, SSP2-4.5, SSP3-7.0, SSP5-8.5), unravels the mechanisms of O3 formation and the impact of isoprene on O3 production using an observation-based box model. Our observation results showed that O3 concentrations were lower in 2020 compared to 2019. The box model analysis suggests a shift in O3 formation from a VOC-limited regime in 2019 to a transition regime in 2020, primarily due to a significant reduction in anthropogenic emissions. Isoprene photochemistry contributed to 7% and 11% of the daytime average net O3 production rates in 2019 and 2020, respectively. The increase can be attributed to a notable rise in RO2 radicals, from 14% in 2019 to 19% in 2020. Under the future scenario with the lowest projected anthropogenic emissions (SSP1-2.6), isoprene-derived RO2 radicals (generated through isoprene oxidation) are expected to account for 36% of the total RO2 radicals. We also use a quasi-EKMA diagram to illustrate the contribution of isoprene to O3 concentrations, highlighting the nonlinear amplification or reduction of its contribution depending on changes in anthropogenic VOCs and NOx concentrations. This nonlinear relationship is influenced by NOx concentrations, with the impact of isoprene being reduced at lower NOx levels. To effectively mitigate long-term O3 pollution, especially given the growing contribution of biogenic precursors, it is crucial to focus on reducing NOx emissions.

Unveiling Trade-Off and Synergy in Simultaneous Removal of NOx, CO, and NH3 on Mixed Metal Oxide Nanostructure Catalysts.

The simultaneous removal reaction (SRR) is a pioneering approach for achieving the simultaneous removal of anthropogenic NOx and CO pollutants through catalytic reactions. To facilitate this removal across diverse industrial fields, it is crucial to understand the trade-offs and synergies among the multiple reactions involved in the SRR process. In this study, we developed mixed metal oxide nanostructures derived from layered double hydroxides as catalysts for the SRR, achieving high catalytic conversions of 93.4, 100, and 91.6% for NOx, CO, and NH3, respectively, at 225 °C. Furthermore, we elucidated the reaction mechanisms, revealing the trade-offs and synergies between the multiple reactions. In addition, we fabricated sheet-type catalysts and conducted SRR tests in a semibench-scale reactor with a gas flow rate of 10 L min-1 at 1% CO concentration. The fabricated catalysts exhibited high SRR activity and stability, even in the presence of SO2, highlighting their potential for practical applications.

The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau.

Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (J1.7) is 2.6 cm-3 s-1, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 105 cm-3). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 106 and 3.7 × 106 cm-3, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NOx via RO2+NO terminations or NO3-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NOx-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.

Uncertainties of biogenic VOC emissions caused by land cover data and implications on ozone mitigation strategies for the Yangtze river Delta region

Biogenic volatile organic compounds (BVOC) play a crucial role in ground-level ozone formation, yet emission quantification faces considerable uncertainties stemming from input data. Land cover data, which determines the distribution of growth forms, is an essential driving input of BVOC emissions. This study explores the uncertainty in BVOC emission estimates arising from using two land cover datasets, specifically the MODIS and ESA land cover data, and the implications for ozone mitigation strategies in the Yangtze River Delta (YRD) region. By employing the MEGAN model for the year 2021, we estimated that ESA land cover data, with a finer 10 m resolution, yields a total BVOC emission estimate of 2299 Gg, which is over 52.9% higher than the MODIS dataset with a resolution of 500 m, attributed to the higher tree coverage (33.9% in ESA vs. 17.6% in MODIS) identified in the ESA dataset. We then simulated the ozone concentrations by both emission estimates with the WRF-CMAQ model. The elevated BVOC emissions based on the ESA data improved the underestimation of simulated isoprene concentrations and consequently resulted in more than 30% higher domain-averaged MDA8 ozone concentration compared to the MODIS-derived BVOC emission. Regarding ozone mitigation strategy, simulation with the ESA-based BVOC emissions results in 0.3–1.2 μg/m3 less ozone reductions compared to that with the MODIS-based emissions when reducing anthropogenic VOC emissions, but 0.7–2.9 μg/m3 higher ozone reductions when controlling anthropogenic NOx emissions. These disparities are more pronounced at the city level, highlighting the importance of accurate BVOC emission estimates for effective ozone control strategies.

The reward and penalty for ozone pollution control caused by natural sources and regional transport: A case study in Guangdong province

Ground-level O3 pollution in the Pearl River Delta region (PRD) is closely related to anthropogenic, natural emissions and regional transport. However, the interactions among different sources and natural intervention in modulating anthropogenic management have not been comprehensively assessed. Here, the WRF-CMAQ-MEGAN modeling system was utilized to simulate an O3 episode over PRD. The integrated source apportionment method (ISAM) and brute-force top-down combined with factor separation approach (BF-TD-FSA) were applied to quantify source contributions, impacts of individual or multiple sources on O3, and decouple interactions among various emissions; additionally, based on ISAM, O3 isopleths visualized MDA8 O3 response of different source types to anthropogenic perturbations. ISAM concluded considerable MDA8 O3 contributions of regional transport in PRD/NPRD (non-PRD areas in Guangdong province) (38.8 %/35.7 %), followed by anthropogenic (32.7 %/24.8 %), BVOC (biogenic volatile organic compounds, 23.8 %/20.3 %) and SNO (soil NO, ∼4 %) emissions. Compared to concentrated anthropogenic contributions, widespread natural contributions were observed across their source areas and along the transport pathways. The BF-TD also revealed that regional transport had the largest impact (>90 μg m−3) on MDA8 O3 while anthropogenic and BVOC emissions greatly affected downwind PRD (64.5 and 7.7 μg m−3). Negative synergy between anthropogenic and natural emissions (especially BVOC emission) suggested potential natural-induced intensification of anthropogenic impact during O3 management. The MDA8 O3 isopleths further demonstrated significant BVOC-induced reward and regional transport-induced penalty for anthropogenic NOx (ANOx) emission control benefits, leading to additional maximum MDA8 O3 decrease and increase by −27.5 and 13.8 μg m−3 in polluted high-emission grids. The natural-induced reward effect could impose loose requirements on anthropogenic reduction (decreased by 13.3 %–17.7 %) if there were no regional transport-induced control penalty. It is advisable to prioritize ANOx control and seek collaboration on air quality management with neighboring provinces to maximize the natural-induced control reward and achieve desired targets with minimal human efforts.

Global estimates of ambient NO2 concentrations and long-term health effects during 2000–2019

High concentrations of ambient NO2 causes serious air pollution and could also pose great threats to human health. However, the long-term trends (20-year) and potential health effects of ambient NO2 exposure globally still shows high uncertainties. In this work, the field measurements, satellite dataset, GEOS-Chem output, and multiple geographical covariates were incorporated into the multi-stage model to investigate the global evolutions of ambient NO2 during 2000–2019. The results indicated that the cross-validation (CV) R2 values of ambient NO2 based on multi-stage model displayed satisfied performance (R2 = 0.78), which was superior to the individual model. Besides, the out-of-bag R2 was 0.75, which suggested the multi-stage model showed the better transferability. At the spatial scale, the NO2 concentrations followed the order of China (16.9 ± 9.0 μg/m3) > India (15.5 ± 5.6 μg/m3) > United States (10.7 ± 5.6 μg/m3) > Europe (7.7 ± 4.5 μg/m3), which was in consistent with the anthropogenic NOx emission. At the temporal scale, the ambient NO2 levels in China experienced persistent increases (0.29 μg/m3/year) during 2000–2013, whereas they showed slight decreases (−0.23 μg/m3/year) during 2013–2019. The ambient NO2 levels in the United States experienced continuous decreases during 2000–2019 (−0.20 μg/m3/year), while both of India and Europe remained relatively stable. Long-term NO2 exposure inevitably increased premature mortalities. The global premature all-cause mortalities associated with the excessive NO2 exposure increased from 288,169 (95% CI: 43,650, 527,971) to 461,301 (95% CI: 69,973, 843,996) in the past 20 years. This study would provide sufficient policy support for future ambient NO2 mitigation.

Traceability and policy suggestions for ozone pollution in heavy industrial city in Northeast China.

In the heavy industrial city of Northeast China, there has been a significant decrease in particulate matter pollution while experiencing a sharp increase in ozone (O3) pollution. However, the main influencing factors and source contributions to O3 remain unclear. Taking the case of Siping as an example, this study analyzed the spatiotemporal characteristics, assessed local source contributions to O3, and revealed regional transmission effects using numeric simulation and statistical methods. Temporally, higher O3 concentrations were observed in summer and the afternoon, with hourly peaks up to 254µg/m3. Spatially, O3 pollution was mainly contributed by background concentrations (34.52%), external transport (34.50%), and local emissions (30.98%) during the case study period (June 11-18, 2021). Among the local emission sources, biological emissions, the industrial sector, and the traffic sector accounted for 35.30%, 32.09%, and 23.58% of the O3 concentration, respectively. For regional atmospheric transmission, high O3 pollution was accompanied by wind from the southwest directions, and the trajectory of air mass transport suggests that eastern Mongolia, the Korean Peninsula, and its neighboring regions contribute to O3 pollution. Furthermore, sensitivity analysis showed that O3 pollution in Siping is a co-controlled region by anthropogenic volatile organic compounds (AVOCs) and NOX, which implies control in an optimal ratio of VOCs and NOX emissions. Thus, our results highlight the importance of joint prevention and control of O3 pollution in the region, optimization of biogenic landscape ecology, and control of VOCs and NOx in both the industrial and transport sectors.

Impacts of global biogenic isoprene emissions on surface ozone during 2000–2019

Biogenic isoprene is an important precursor of tropospheric ozone (O3). Here, a coupled chemistry–vegetation model was used to quantify the contributions of isoprene emissions to surface O3 pollution on the global scale during 2000–2019. The biogenic isoprene emissions showed high values in mid–low latitudes and seasonal peaks in the summer hemispheres. They promote global surface O3 concentrations by 1.75 ppbv annually with regional hotspots of 4.39 ppbv (8.8%) in China and 5.36 ppbv (11.1%) in the U.S. in boreal summer. In the past two decades, isoprene emissions increased by 1.32 TgC yr−1 (0.67% yr−1) in the Northern Hemisphere but decreased by 0.71 TgC yr−1 (0.44% yr−1) in the Southern Hemisphere. Such changes of isoprene made opposite contributions to the surface O3 trend, with 0.26 ppbv yr−1 in eastern China but −0.32 ppbv yr−1 in the southeastern U.S. due to the changes in the background regime of chemical reactions. The impact of anthropogenic changes on the O3 trend is consistent with that of biogenic isoprene, but two to four times stronger in magnitude. This study revealed that the effective control of anthropogenic NOx emissions could mitigate regional O3 pollution even with the increased isoprene emissions under global warming.

A quantitative analysis of causes for increasing ozone pollution in Shanghai during the 2022 lockdown and implications for control policy

Ground-level ozone (O3) pollution is a major air quality issue in densely populated urban areas. Despite a significant decline in human activities in the megacity Shanghai from March 28 to May 31, 2022, ground-level measurements indicate a rise in maximum daily average 8-h (MDA8) O3 concentrations in comparison to the corresponding period in 2021. There is a need for quantitative analysis to identify the reasons behind this increasing O3 concentration. We analyzed ground measurements of O3 and its precursors and meteorological parameters made in Shanghai, using random-forest (RF) model and chemical box model to elucidate the roles of meteorological and chemical factors in influencing O3 concentrations. Across urban, suburban, semi-rural, and coastal sites, the urban center of Shanghai experienced the largest decreases in the concentrations of nitrogen oxides (NOx; 53%) and volatile organic compounds (VOCs; 52%), with the most notable rise in MDA8 O3 concentrations (16%). RF modeling indicates that meteorological factors reduced MDA8 O3 concentrations by a marginal 3%, whereas a decline in anthropogenic emissions resulted in a 17% increase in MDA8 O3 concentrations. Chemical box modeling at the Pudong urban site indicates that while the decline in VOCs reduced O3 production by 42%, this was negated by a reduction in NOx from traffic emissions, which enhanced O3 production by 51%, resulting in an increase in O3 production overall. Despite a halving in precursor levels, Shanghai's urban centre remains predominately under VOC-limited conditions throughout the study period, with high NO2 levels from the petrochemical industry and traffic emissions. Joint control of anthropogenic VOCs (AVOCs) and NOx, with a ratio greater than 1.29, could help avoid exacerbation of O3 pollution and reduce NO2 pollution. Our findings emphasize the necessity of reducing industrial emissions along with ongoing green transportation strategies for alleviating O3 pollution in megacities like Shanghai.

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.

Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies

Abstract. Lightning is one of the primary natural sources of nitric oxide (NO), and the influence of lightning-induced NO (LNO) emission on air quality has been investigated in the past few decades. In the current study an LNO emissions model, which derives LNO emission estimates from satellite-observed lightning optical energy, is introduced. The estimated LNO emission is employed in an air quality modeling system to investigate the potential influence of LNO on tropospheric ozone. Results show that lightning produced 0.174 Tg N of nitrogen oxides (NOx = NO + NO2) over the contiguous US (CONUS) domain between June and September 2019, which accounts for 11.4 % of the total NOx emission. In August 2019, LNO emission increased ozone concentration within the troposphere by an average of 1 %–2 % (or 0.3–1.5 ppbv), depending on the altitude; the enhancement is maximum at ∼ 4 km above ground level and minimum near the surface. The southeastern US has the most significant ground-level ozone increase, with up to 1 ppbv (or 2 % of the mean observed value) difference for the maximum daily 8 h average (MDA8) ozone. These numbers are near the lower bound of the uncertainty range given in previous studies. The decreasing trend in anthropogenic NOx emissions over the past 2 decades increases the relative contribution of LNO emissions to total NOx emissions, suggesting that the LNO production rate used in this study may need to be increased. Corrections for the sensor flash detection efficiency may also be helpful. Moreover, the episodic impact of LNO on tropospheric ozone can be considerable. Performing backward trajectory analyses revealed two main reasons for significant ozone increases: long-distance chemical transport and lightning activity in the upwind direction shortly before the event.

Improved Spatial Resolution in Modeling of Nitrogen Oxide Concentrations in the Los Angeles Basin.

The extent to which emission control technologies and policies have reduced anthropogenic NOx emissions from motor vehicles is large but uncertain. We evaluate a fuel-based emission inventory for southern California during the June 2021 period, coinciding with the Re-Evaluating the Chemistry of Air Pollutants in CAlifornia (RECAP-CA) field campaign. A modified version of the Fuel-based Inventory of Vehicle Emissions (FIVE) is presented, incorporating 1.3 km resolution gridding and a new light-/medium-duty diesel vehicle category. NOx concentrations and weekday-weekend differences were predicted using the WRF-Chem model and evaluated using satellite and aircraft observations. Model performance was similar on weekdays and weekends, indicating appropriate day-of-week scaling of NOx emissions and a reasonable distribution of emissions by sector. Large observed weekend decreases in NOx are mainly due to changes in on-road vehicle emissions. The inventory presented in this study suggests that on-road vehicles were responsible for 55-72% of the NOx emissions in the South Coast Air Basin, compared to the corresponding fraction (43%) in the planning inventory from the South Coast Air Quality Management District. This fuel-based inventory suggests on-road NOx emissions that are 1.5 ± 0.4, 2.8 ± 0.6, and 1.3 ± 0.7 times the reference EMFAC model estimates for on-road gasoline, light- and medium-duty diesel, and heavy-duty diesel, respectively.

Exploring Deposition Observations of Oxidized Sulfur and Nitrogen as a Constraint on Emissions in the United States

AbstractEmissions of anthropogenic sulfur and nitrogen oxides form secondary pollutants that impact human health, ecosystems, and climate. Accurate estimates of emissions trends are needed to verify the effectiveness of the regulation of these species. We explore the utility of deposition measurements of SOx (=SO2 + SO42−) and TNO3 (=HNO3 + NO3−) as constraints on emissions trends of SOx and NOx in the conterminous United States (CONUS) from 1990 to 2021. The GEOS‐Chem model captures observed annual SOx and TNO3 wet deposition at NADP‐NTN sites in 2011 with a −15% and +15% normalized mean bias (NMB), respectively. The model overestimates the dry deposition of SOx and TNO3 estimated at CASTNET sites in 2011 (NMB >100%), however, this bias is substantially reduced when using an alternate derived dry deposition data set at the same sites, highlighting the uncertainty in dry deposition velocities. Despite this, we find that the model (driven by scaled NEI emissions) captures the relative trend in dry deposition of SOx (−93% observed and −94% simulated) and TNO3 (−66% observed and −68% simulated) from 1990 to 2021 and that these decreases closely reflect the trends in anthropogenic SO2 emissions (−93%) and anthropogenic NOx emissions (−71%), respectively. SOx and TNO3 wet deposition observations are dominated by soluble secondary products and are more influenced by natural and transboundary sources, and therefore have decreased more modestly over the same period (−78% and −52%). Natural sources of NOx are relatively constant during this time and therefore moderate the reduction in total NOx emissions (−55%).

Impacts of changes in climate, land use, and emissions on global ozone air quality by mid-21st century following selected Shared Socioeconomic Pathways

Surface ozone (O3) is a major air pollutant and greenhouse gas with significant risks to human health, vegetation, and climate. Uncertainties around the impacts of various critical factors on O3 is crucial to understand. We used the Community Earth System Model to investigate the impacts of land use and land cover change (LULCC), climate, and emissions on global O3 air quality under selected Shared Socioeconomic Pathways (SSPs). Our findings show that increasing forest cover by 20 % under SSP1 in East China, Europe, and the eastern US leads to higher isoprene emissions leading 2–5 ppb increase in summer O3 levels. Climate-induced meteorological changes, like rising temperatures, further enhance BVOC emissions and increase O3 levels by 10–20 ppb in urban areas with high NOx levels. However, higher BVOC emissions can reduce O3 levels by 5–10 ppb in remote environments. Future NOx emissions control reduces O3 levels by 5–20 ppb in the US and Europe in all SSPs, but reductions in NOx and changes in oxidant titration increase O3 in southeast China in SSP5. Increased NOx emissions in southern Africa and India significantly elevate O3 levels up to 15 ppb under different SSPs. Climate change is equally important as emissions changes, sometimes countering the benefits of emissions control. The combined effects of emissions, climate, and land cover result in worse O3 air quality in northern India (+40 %) and East China (+20 %) under SSP3 due to anthropogenic NOx and climate-induced BVOC emissions. Over the northern hemisphere, surface O3 decreases due to reduced NOx emissions, although climate and land use changes can increase O3 levels regionally. By 2050, O3 levels in most Asian regions exceed the World Health Organization safety limit for over 150 days per year. Our study emphasizes the need to consider complex interactions for effective air pollution control and management in the future.

Enhanced summertime background ozone by anthropogenic emissions – Implications on ozone control policy and health risk assessment

Quantifying background ozone (O3-BG) is critical for emission control policy development due to its significant contribution to the overall O3 levels. However, O3-BG is still hard to monitor because of the universal existence of human activities and the complex interactions between anthropogenic and biogenic emissions. Here, we used a source-oriented chemical transport model to assess O3-BG with (O3-BG-anth) and without (O3-BG-ult) the presence of anthropogenic emissions. Results show that anthropogenic emissions enhance O3-BG-anth compared to that derived from biogenic emissions alone (O3-BG-ult). The enhancement increases with increasing O3 levels because anthropogenic emissions generally increase abundance of OH and HO2 radicals, raising atmospheric oxidation capacity. Sensitivity analysis demonstrates that anthropogenic NOx abatement could have the co-benefit of reducing biogenic O3, leading to more effective O3 pollution control. In contrast, reducing anthropogenic VOCs increases the production of biogenic O3, which is not beneficial to overall O3 reduction. Our findings provide valuable information for developing emission control policy and risk assessment.

Integrated analysis of the transport process and source attribution of an extreme ozone pollution event in Hefei at different vertical heights: A case of study

The Yangtze River Delta (YRD) region frequently experiences ozone pollution events during the summer and autumn seasons. High-concentration events are typically related to synoptic weather patterns, which impact the transport and photochemical production of ozone at multiple scales, ranging from the local to regional scale. To better understand the regional ozone pollution problem, studies on ozone source attribution are needed, especially regarding the contributions of sources at different vertical heights based on tagging the region or time periods. Between September 3 and 8, 2020, an episode of ozone concentration anomaly high was observed in Hefei through ground-based stations and ozone Lidar. The mechanism behind this event was uncovered through synoptic weather pattern analysis and using the Weather Research and Forecasting Chemistry model (WRF-Chem). Because an approaching typhoon caused variable wind direction, the O3-rich air masses (ORMs) arising from the YRD region were transported to Hefei via the nocturnal residual layer and descended to the ground through horizontal advection and vertical mixing processes the next day. Based on geographic source tagging, the anthropogenic NOx emissions (ANEs) from local and regional sources were the main contributors to the heavy ozone pollution over Hefei on September 6. Furthermore, the intra-regional transported ozone from southern Jiangsu (SJS), southern Anhui (SAH), and Zhejiang (ZJ) in the YRD was the main driving factor of the surface and upper atmosphere ozone pollution. Based on time period tagging, The ozone generated due to ANEs from September 3 to 5 significantly contributed to this episode. It is important to pay attention to the impact of ANEs on September 5 on the surface peak ozone concentration the following day (i.e., September 6). Our findings provide significant insights into the regional ozone transport mechanism in the YRD and optimization of measures to prevent and control heavy ozone pollution on spatiotemporal scales.

Space-Based Observations of Ozone Precursors within California Wildfire Plumes and the Impacts on Ozone-NOx-VOC Chemistry.

The frequency of wildfires in the western United States has escalated in recent decades. Here we examine the impacts of wildfires on ground-level ozone (O3) precursors and the O3-NOx-VOC chemistry from the source to downwind urban areas. We use satellite retrievals of nitrogen dioxide (NO2) and formaldehyde (HCHO, an indicator of VOC) from the Tropospheric Monitoring Instrument (TROPOMI) to track the evolution of O3 precursors from wildfires over California from 2018 to 2020. We improved these satellite retrievals by updating the a priori profiles and explicitly accounting for the effects of smoke aerosols. TROPOMI observations reveal that the extensive and intense fire smoke in 2020 led to an overall increase in statewide annual average HCHO and NO2 columns by 16% and 9%. The increase in the level of NO2 offsets the anthropogenic NOx emission reduction from the COVID-19 lockdown. The enhancement of NO2 within fire plumes is concentrated near the regions actively burning, whereas the enhancement of HCHO is far-reaching, extending from the source regions to urban areas downwind due to the secondary production of HCHO from longer-lived VOCs such as ethene. Consequently, a larger increase in NOx occurs in NOx-limited source regions, while a greater increase in HCHO occurs in VOC-limited urban areas, both contributing to more efficient O3 production.