Changes In Nitrogen Oxides Emissions Research Articles

Cropland soil nitrogen oxide emissions vary with dairy manure incorporation methods

AbstractSoils contribute 15%–75% of total atmospheric nitrogen oxide (NOx) emissions in agricultural regions during the growing season. However, the impacts of cropland fertilizer management on spatially heterogeneous, temporally episodic NOx emission patterns are highly uncertain. We examine the effects of liquid slurry dairy manure application practices on soil NOx emissions in rainfed, corn‐soybean rotations during spring 2016 and 2017. Daily soil NOx emissions and weekly soil inorganic N measurements were performed in a randomized split–split plot design for 1–4 weeks following manure applications. NOx emissions and soil N with shallow‐disk injection and chisel‐disk manure incorporation methods were compared with unincorporated broadcast practices. Injected manure and chisel‐disk incorporation exhibited two–four times larger mean NOx emissions than those with unincorporated broadcast manure. Larger soil NOx emissions with manure incorporation practices were driven by the predominance of nitrification in these treatments with evidence of soil nitrate production. Soil NOx emission differences between treatments were detectable across order of magnitude changes in daily NOx emissions during two growing seasons. Larger soil NOx emissions associated with manure incorporation practices compared with unincorporated broadcast practices occur alongside larger N2O and smaller NH3 emissions, highlighting important air quality and climate impact tradeoffs for cropland manure fertilizer management choices.

Emissions of NOx from blending of hydrogen and natural gas in space heating boilers

As part of climate change commitments, the United Kingdom is considering an incremental transition from natural gas to hydrogen for domestic heating, blending up to 20% of hydrogen (by volume) into the national gas network. We consider the possible impacts of this policy on nitrogen oxides (NOx) emissions, a minor waste by-product from combustion. A meta-analysis of changes in NOx emissions from hydrogen/natural gas blends used in gas burners is undertaken, with focus on mixtures between 5% and 20% v/v. Literature reports are highly variable: for a 5% hydrogen blend, changes in NOx emissions, when compared to burning pure natural gas, vary over the range –12% to +39%, with a mean change across 14 studies of +8%. These estimates required an important assumption to be made that, when not explicitly described, all literature data on changes in NOx emissions and/or concentrations were suitably corrected for the reduced energy density and heat output arising once hydrogen is added. A NOx increase can be rationalized through the increased adiabatic flame temperature generated from hydrogen combustion. The associated range of plausible damage costs of a 5% hydrogen blend is estimated to fall within the range –117 million GBP to +362 million GBP per year; 20% hydrogen (the maximum that could be accommodated with existing infrastructure) would lead to a change in emissions in the range –50 to +154% with a change in damage costs of between –467 million GBP and +1,146 million GBP per year. The mean change is estimated at 292 million GBP per year. For existing poor performing boilers, an economic case can be made for scrappage and replacement based primarily on NOx damage costs avoided. The response of older boilers to added hydrogen is a critical evidence gap that needs filling before further decisions on hydrogen as a heating fuel are made.

Decadal Variabilities in Tropospheric Nitrogen Oxides Over United States, Europe, and China

AbstractGlobal trends in tropospheric nitrogen dioxide (NO2) have changed dramatically in the past decade. Here, we investigate tropospheric NO2 variabilities over United States, Europe, and E. China in 2005–2018 to explore the mechanisms governing the variation of this critical pollutant. We found large uncertainties in the trends of anthropogenic nitrogen oxides (NOx) emissions, for example, the reductions of NOx emissions, derived with different approaches and data sets, are in the range of 35%–50% over the United States and 15%–45% over Europe in 2005–2018. By contrast, the analysis in this work indicates declines of anthropogenic NOx emissions by about 40% and 25% over the United States and Europe, respectively, in 2005–2018, and about 20% over E. China in 2012–2018. However, the shift of major NOx sources from power generation to industrial and transportation sectors has led to noticeable diminishing effects in emission controls. Furthermore, satellite measurements exhibit the influence of NO2 background levels over the United States and Europe, which offset the impacts of anthropogenic emission declines, resulting in flatter trends of tropospheric NO2 over the United States and Europe. Our analysis further reveals underestimation of background NO2 by chemical transport models, which can lead to inaccurate interpretations of satellite measurements. We use surface in‐situ NO2 observations to diagnose the satellite‐observed NO2 trends and find top‐down NOx emissions over urban grids represent the changes in anthropogenic NOx emissions better. This work highlights the importance of comprehensive applications of different analysis approaches to better characterizing atmospheric composition evolution.

Changes in Power Plant NOx Emissions over Northwest Greece Using a Data Assimilation Technique

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).

Assessment of pre-industrial to present-day anthropogenic climate forcing in UKESM1

Abstract. Quantifying forcings from anthropogenic perturbations to the Earth system (ES) is important for understanding changes in climate since the pre-industrial (PI) period. Here, we quantify and analyse a wide range of present-day (PD) anthropogenic effective radiative forcings (ERFs) with the UK's Earth System Model (ESM), UKESM1, following the protocols defined by the Radiative Forcing Model Intercomparison Project (RFMIP) and the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). In particular, quantifying ERFs that include rapid adjustments within a full ESM enables the role of various chemistry–aerosol–cloud interactions to be investigated. Global mean ERFs for the PD (year 2014) relative to the PI (year 1850) period for carbon dioxide (CO2), nitrous oxide (N2O), ozone-depleting substances (ODSs), and methane (CH4) are 1.89 ± 0.04, 0.25 ± 0.04, −0.18 ± 0.04, and 0.97 ± 0.04 W m−2, respectively. The total greenhouse gas (GHG) ERF is 2.92 ± 0.04 W m−2. UKESM1 has an aerosol ERF of −1.09 ± 0.04 W m−2. A relatively strong negative forcing from aerosol–cloud interactions (ACI) and a small negative instantaneous forcing from aerosol–radiation interactions (ARI) from sulfate and organic carbon (OC) are partially offset by a substantial forcing from black carbon (BC) absorption. Internal mixing and chemical interactions imply that neither the forcing from ARI nor ACI is linear, making the aerosol ERF less than the sum of the individual speciated aerosol ERFs. Ozone (O3) precursor gases consisting of volatile organic compounds (VOCs), carbon monoxide (CO), and nitrogen oxides (NOx), but excluding CH4, exert a positive radiative forcing due to increases in O3. However, they also lead to oxidant changes, which in turn cause an indirect aerosol ERF. The net effect is that the ERF from PD–PI changes in NOx emissions is negligible at 0.03 ± 0.04 W m−2, while the ERF from changes in VOC and CO emissions is 0.33 ± 0.04 W m−2. Together, aerosol and O3 precursors (called near-term climate forcers (NTCFs) in the context of AerChemMIP) exert an ERF of −1.03 ± 0.04 W m−2, mainly due to changes in the cloud radiative effect (CRE). There is also a negative ERF from land use change (−0.17 ± 0.04 W m−2). When adjusted from year 1850 to 1700, it is more negative than the range of previous estimates, and is most likely due to too strong an albedo response. In combination, the net anthropogenic ERF (1.76 ± 0.04 W m−2) is consistent with other estimates. By including interactions between GHGs, stratospheric and tropospheric O3, aerosols, and clouds, this work demonstrates the importance of ES interactions when quantifying ERFs. It also suggests that rapid adjustments need to include chemical as well as physical adjustments to fully account for complex ES interactions.

Enhanced atmospheric oxidation capacity and associated ozone increases during COVID-19 lockdown in the Yangtze River Delta

Aggressive air pollution control in China since 2013 has achieved sharp decreases in fine particulate matter (PM2.5), along with increased ozone (O3) concentrations. Due to the pandemic of coronavirus disease 2019 (COVID-19), China imposed nationwide restriction, leading to large reductions in economic activities and associated emissions. In particular, large decreases were found in nitrogen oxides (NOx) emissions (>50%) from transportation. However, O3 increased in the Yangtze River Delta (YRD), which cannot be fully explained by changes in NOx and volatile organic compound (VOCs) emissions. In this study, the Community Multi-scale Air Quality model was used to investigate O3 increase in the YRD. Our results show a significant increase of atmospheric oxidation capacity (AOC) indicated by enhanced oxidants levels (up to +25%) especially in southern Jiangsu, Shanghai and northern Zhejiang, inducing the elevated O3 during lockdown. Moreover, net P(HOx) of 0.4 to 1.6 ppb h−1 during lockdown (Case 2) was larger than the case without lockdown (Case 1), mainly resulting in the enhanced AOC and higher O3 production rate (+12%). This comprehensive analysis improves our understanding on AOC and associated O3 formation, which helps to design effective strategies to control O3.

The changing role of organic nitrates in the removal and transport of NO<sub><i>x</i></sub>

Abstract. A better understanding of the chemistry of nitrogen oxides (NOx) is crucial to effectively reducing air pollution and predicting future air quality. The response of NOx lifetime to perturbations in emissions or in the climate system is set in large part by whether NOx loss occurs primarily by the direct formation of HNO3 or through the formation of alkyl and multifunctional nitrates (RONO2). Using 15 years of detailed in situ observations, we show that in the summer daytime continental boundary layer the relative importance of these two pathways can be well approximated by the relative likelihood that OH will react with NO2 or instead with a volatile organic compound (VOC). Over the past decades, changes in anthropogenic emissions of both NOx and VOCs have led to a significant increase in the overall importance of RONO2 chemistry to NOx loss. We find that this shift is associated with a decreased effectiveness of NOx emissions reductions on ozone production in polluted areas and increased transport of NOx from source to receptor regions. This change in chemistry, combined with changes in the spatial pattern of NOx emissions, is observed to be leading to a flatter distribution of NO2 across the United States, potentially transforming ozone air pollution from a local issue into a regional one.

Effect of Urbanization on Ozone and Resultant Health Effects in the Pearl River Delta Region of China

AbstractThe United Nations has reported that 55% of the global population resides in urban areas, and 68% of the population is expected to be urban dwellers by 2050. Urbanization has critical implications for global land cover. Relevant literature has provided evidence attributing climatic effects to urban expansion; however, few studies have investigated the effect on public health and pollutant sensitivity to emissions. This study aimed to characterize the effect of urbanization‐induced changes in regional climate on ozone (O3), to evaluate ozone sensitivity to nitrogen oxide (NOx) and volatile organic compound (VOC) emissions, and to estimate premature mortalities due to O3 exposure. We employed atmospheric models with the higher‐order decoupled direct method to simulate effects of urbanization on O3 and to determine O3 sensitivity to NOx and VOC emissions. China‐specific concentration response functions were utilized to estimate cardiovascular and respiratory mortalities due to ozone exposure. Urbanization increased O3, which translated to a 39.6% increase in O3‐induced premature mortality (1,100 deaths). Moreover, O3 has become less/more sensitive to unit changes in NOx and VOC emissions in various cities. Urban greening may reduce urban temperature, but it may increase O3 in some cities due to the additional VOC emissions of greening. These findings highlight the strong interactions between land use policies, urban climate adaptation strategies, and air quality policies, suggesting the need of cobeneficial strategies and policies. We proposed a precision environmental management concept that emphasizes the importance of considering the specific atmospheric condition and composition of a city when formulating its environmental policies.

Productivity Spillovers From Pollution Reduction: Reducing Coal Use Increases Crop Yields

Air pollution reduces crop yields by slowing down photosynthesis. We estimate the increase in US corn and soybean yields attributed to the recent dramatic reductions in emissions of nitrogen oxides (NOx) from electric power plants. In response to the observed changes in power plant NOx emissions over the eight‐year period from 2003–05 to 2011–13, we estimate that average corn yields improved by 2.46% and soybean yields by 1.62%. These improvements imply an increase in total surplus of $1.60 billion annually across the two crops. The estimated yield improvements vary substantially across states depending on the change in NOx emissions. For corn, they range from 0.32% to 6.87% and for soybeans, they range from 0.21% to 4.30%. The demand for the two crops is quite inelastic, which means that prices decrease by more than production increases in response to this positive productivity shock and the implied rightward shift of the crop supply curve. Due to the low elasticities of supply and demand for U.S. corn and soybeans, we conclude from a welfare analysis that these changes made consumers better off and farmers worse off.

Response of winter fine particulate matter concentrations to emission and meteorology changes in North China

Abstract. The winter haze is a growing problem in North China, but the causes are not well understood. The chemistry version of the Weather Research and Forecasting model (WRF-Chem) was applied in North China to examine how PM2.5 concentrations change in response to changes in emissions (sulfur dioxide (SO2), black carbon (BC), organic carbon (OC), ammonia (NH3), and nitrogen oxides (NOx)), as well as meteorology (temperature, relative humidity (RH), and wind speeds) changes in winter. From 1960 to 2010, the dramatic changes in emissions lead to +260 % increases in sulfate, +320 % increases in nitrate, +300 % increases in ammonium, +160 % increases in BC, and +50 % increases in OC. The responses of PM2.5 to individual emission species indicate that the simultaneous increases in SO2, NH3, and NOx emissions dominated the increases in PM2.5 concentrations. PM2.5 shows more notable increases in response to changes in SO2 and NH3 as compared to increases in response to changes in NOx emissions. In addition, OC also accounts for a large fraction in PM2.5 changes. These results provide some implications for haze pollution control. The responses of PM2.5 concentrations to temperature increases are dominated by changes in wind fields and mixing heights. PM2.5 shows relatively smaller changes in response to temperature increases and RH decreases compared to changes in response to changes in wind speed and aerosol feedbacks. From 1960 to 2010, aerosol feedbacks have been significantly enhanced due to higher aerosol loadings. The discussions in this study indicate that dramatic changes in emissions are the main cause of increasing haze events in North China, and long-term trends in atmospheric circulations may be another important cause since PM2.5 is shown to be substantially affected by wind speed and aerosol feedbacks. More studies are necessary to get a better understanding of the aerosol–circulation interactions.

Impact of the 2008 Global Recession on air quality over the United States: Implications for surface ozone levels from changes in NOx emissions

AbstractSatellite and ground observations detected large variability in nitrogen oxides (NOx) during the 2008 economic recession, but the impact of the recession on air quality has not been quantified. This study combines observed NOx trends and a regional chemical transport model to quantify the impact of the recession on surface ozone (O3) levels over the continental United States. The impact is quantified by simulating O3 concentrations under two emission scenarios: business‐as‐usual (BAU) and recession. In the BAU case, the emission projection from the Cross‐State Air Pollution Rule is used to estimate the “would‐be” NOx emission level in 2011. In the recession case, the actual NO2 trends observed from Air Quality System ground monitors and the Ozone Monitoring Instrument on the Aura satellite are used to obtain “realistic” changes in NOx emissions. The model prediction with the recession effect agrees better with ground O3 observations over time and space than the prediction with the BAU emission. The results show that the recession caused a 1–2 ppbv decrease in surface O3 concentration over the eastern United States, a slight increase (0.5–1 ppbv) over the Rocky Mountain region, and mixed changes in the Pacific West. The gain in air quality benefits during the recession, however, could be quickly offset by the much slower emission reduction rate during the post‐recession period.

Enhancement of aerosol responses to changes in emissions over East Asia by gas‐oxidant‐aerosol coupling and detailed aerosol processes

AbstractWe quantify the responses of aerosols to changes in emissions (sulfur dioxide, black carbon (BC), primary organic aerosol, nitrogen oxides (NOx), and volatile organic compounds) over East Asia by using simulations including gas‐oxidant‐aerosol coupling, organic aerosol (OA) formation, and BC aging processes. The responses of aerosols to NOx emissions are complex and are dramatically changed by simulating gas‐phase chemistry and aerosol processes online. Reduction of NOx emissions by 50% causes a 30–40% reduction of oxidant (hydroxyl radical and ozone) concentrations and slows the formation of sulfate and OA by 20–30%. Because the response of OA to changes in NOx emissions is sensitive to the treatment of emission and oxidation of semivolatile and intermediate volatility organic compounds, reduction of the uncertainty in these processes is necessary to evaluate gas‐oxidant‐aerosol coupling accurately. Our simulations also show that the sensitivity of aerosols to changes in emissions is enhanced by 50–100% when OA formation and BC aging processes are resolved in the model. Sensitivity simulations show that the increase of NOx emissions from 1850 to 2000 explains 70% (40%) of the enhancement of aerosol mass concentrations (direct radiative effects) over East Asia during that period through enhancement of oxidant concentrations and that this estimation is sensitive to the representation of OA formation and BC aging processes. Our results demonstrate the importance of simultaneous simulation of gas‐oxidant‐aerosol coupling and detailed aerosol processes. The impact of NOx emissions on aerosol formation will be a key to formulating effective emission reduction strategies such as BC mitigation and aerosol reduction policies in East Asia.

Simulating the air quality impacts of traffic calming schemes in a dense urban neighborhood

In this study, the effects of isolated traffic calming measures and area-wide calming schemes on air quality in a dense neighborhood were estimated using a combination of microscopic traffic simulation, emission, and dispersion modeling. Results indicated that traffic calming measures did not have as large an effect on nitrogen dioxide (NO2) concentrations as the effect observed on nitrogen oxide (NOx) emissions. Changes in emissions resulted in highly disproportional changes in pollutant levels due to daily meteorological conditions, road geometry and orientation with respect to the wind. Average NO2 levels increased between 0.1% and 10% with respect to the base-case while changes in NOx emissions varied between 5% and 160%. Moreover, higher wind speeds decreased NO2 concentrations on both sides of the roadway. Among the traffic calming measures, speed bumps produced the highest increases in NO2 levels.

Changes in nitrogen oxides emissions in California during 2005–2010 indicated from top‐down and bottom‐up emission estimates

AbstractIn California, emission control strategies have been implemented to reduce air pollutants. Here we estimate the changes in nitrogen oxides (NOx = NO + NO2) emissions in 2005–2010 using a state‐of‐the‐art four‐dimensional variational approach. We separately and jointly assimilate surface NO2 concentrations and tropospheric NO2 columns observed by Ozone Monitoring Instrument (OMI) into the regional‐scale Sulfur Transport and dEposition Model (STEM) chemical transport model on a 12 × 12 km2 horizontal resolution grid in May 2010. The assimilation generates grid‐scale top‐down emission estimates, and the updated chemistry fields are evaluated with independent aircraft measurements during the NOAA California Nexus (CalNex) field experiment. The emission estimates constrained only by NO2 columns, only by surface NO2, and by both indicate statewide reductions of 26%, 29%, and 30% from ~0.3 Tg N/yr in the base year of 2005, respectively. The spatial distributions of the emission changes differ in these cases, which can be attributed to many factors including the differences in the observation sampling strategies and their uncertainties, as well as those in the sensitivities of column and surface NO2 with respect to NOx emissions. The updates in California's NOx emissions reduced the mean error in modeled surface ozone in the Western U.S., even though the uncertainties in some urban areas increased due to their NOx‐saturated chemical regime. The statewide reductions in NOx emissions indicated from our observationally constrained emission estimates are also reflected in several independently developed inventories: ~30% in the California Air Resources Board bottom‐up inventory, ~4% in the 2008 National Emission Inventory, and ~20% in the annual mean top‐down estimates by Lamsal et al. using the global Goddard Earth Observing System (GEOS)‐Chem model and OMI NO2 columns. Despite the grid‐scale differences among all top‐down and bottom‐up inventories, they all indicate stronger emission reductions in the urban regions. This study shows the potential of using space‐/ground‐based monitoring data and advanced data assimilation approach to timely and independently update NOx emission estimates on a monthly scale and at a fine grid resolution. The well‐evaluated results here suggest that these approaches can be applied more broadly.

The climate impact of ship NO<sub>x</sub> emissions: an improved estimate accounting for plume chemistry

Abstract. Nitrogen oxide (NOx) emissions from maritime shipping produce ozone (O3) and hydroxyl radicals (OH), which in turn destroy methane (CH4). The balance between this warming (due to O3) and cooling (due to CH4) determines the net effect of ship NOx on climate. Previous estimates of the chemical impact and radiative forcing (RF) of ship NOx have generally assumed that plumes of ship exhaust are instantly diluted into model grid cells spanning hundreds of kilometers, even though this is known to produce biased results. Here we improve the parametric representation of exhaust-gas chemistry developed in the GEOS-Chem chemical transport model (CTM) to provide the first estimate of RF from shipping that accounts for sub-grid-scale ship plume chemistry. The CTM now calculates O3 production and CH4 loss both within and outside the exhaust plumes and also accounts for the effect of wind speed. With the improved modeling of plumes, ship NOx perturbations are smaller than suggested by the ensemble of past global modeling studies, but if we assume instant dilution of ship NOx on the grid scale, the CTM reproduces previous model results. Our best estimates of the RF components from increasing ship NOx emissions by 1 Tg(N) yr−1 are smaller than that given in the past literature: + 3.4 ± 0.85 mW m−2 (1σ confidence interval) from the short-lived ozone increase, −5.7 ± 1.3 mW m−2 from the CH4 decrease, and −1.7 ± 0.7 mW m−2 from the long-lived O3 decrease that accompanies the CH4 change. The resulting net RF is −4.0 ± 2.0 mW m−2 for emissions of 1 Tg(N) yr−1. Due to non-linearity in O3 production as a function of background NOx, RF from large changes in ship NOx emissions, such as the increase since preindustrial times, is about 20% larger than this RF value for small marginal emission changes. Using sensitivity tests in one CTM, we quantify sources of uncertainty in the RF components and causes of the ±30% spread in past model results; the main source of uncertainty is the composition of the background atmosphere in the CTM, which is driven by model formulation (±10 to 20%) and the plausible range of anthropogenic emissions (±10%).

Detection from space of a reduction in anthropogenic emissions of nitrogen oxides during the Chinese economic downturn

Abstract. Rapid economic and industrial development in China and relatively weak emission controls have resulted in significant increases in emissions of nitrogen oxides (NOx) in recent years, with the exception of late 2008 to mid 2009 when the economic downturn led to emission reductions detectable from space. Here vertical column densities (VCDs) of tropospheric NO2 retrieved from satellite observations by SCIAMACHY, GOME-2 and OMI (both by KNMI and by NASA) are used to evaluate changes in emissions of NOx from October 2004 to February 2010 identifying impacts of the economic downturn. Data over polluted regions of Northern East China suggest an increase of 27–33 % in 12-month mean VCD of NO2 prior to the downturn, consistent with an increase of 49 % in thermal power generation (TPG) reflecting the economic growth. More detailed analysis is used to quantify changes in emissions of NOx in January over the period 2005–2010 when the effect of the downturn was most evident. The GEOS-Chem model is employed to evaluate the effect of changes in chemistry and meteorology on VCD of NO2. This analysis indicates that emissions decreased by 20 % from January 2008 to January 2009, close to the reduction of 18 % in TPG that occurred over the same interval. A combination of three independent approaches indicates that the economic downturn was responsible for a reduction in emissions by 9–11 % in January 2009 with an additional decrease of 10 % attributed to the slow-down in industrial activity associated with the coincident celebration of the Chinese New Year; errors in the estimate are most likely less than 3.4 %.

Estimation of multiyear changes in nitrogen oxide emissions in megalopolises from satellite measurements

The influence that megalopolises have on the atmospheric composition on regional and global scales is the subject of intense investigations; however, data on the emissions of pollutants used for such investigations are often insufficiently reliable. In this work the possibilities for diagnosing long-term changes in nitrogen oxide emissions in megalopolises are investigated based on a combined use of data from satellite measurements and modeling of the tropospheric nitrogen dioxide content. Primary emphasis is placed on analyzing possible situations when emission changes are of a nonlinear character. The proposed methodology includes an original method for the nonlinear approximation of changes in a physical quantity from a noised time series of its measurements. Changes in NOx emissions are investigated in 12 megalopolises of Europe and the Middle East in the period from 1996 to 2008. Statistically significant changes in NOx emissions are detected in five megalopolises (Baghdad, Madrid, Milan, Moscow, and Paris). By using three megalopolises (Madrid, Milan, and Paris) as an example, it is shown that a nonlinear approximation of NOx emission changes agrees better with independent ground-based measurements than an analogous linear approximation.

Application of satellite observations for timely updates to global anthropogenic NOxemission inventories

[1] Anthropogenic emissions of nitrogen oxides (NOx) can change rapidly due to economic growth or control measures. Bottom-up emissions estimated using source-specific emission factors and activity statistics require years to compile and can become quickly outdated. We present a method to use satellite observations of tropospheric NO2 columns to estimate changes in NOx emissions. We use tropospheric NO2 columns retrieved from the SCIAMACHY satellite instrument for 2003–2009, the response of tropospheric NO2 columns to changes in NOx emissions determined from a global chemical transport model (GEOS-Chem), and the bottom-up anthropogenic NOx emissions for 2006 to hindcast and forecast the inventories. We evaluate our approach by comparing bottom-up and hindcast emissions for 2003. The two inventories agree within 6.0% globally and within 8.9% at the regional scale with consistent trends in western Europe, North America, and East Asia. We go on to forecast emissions for 2009. During 2006–2009, anthropogenic NOx emissions over land increase by 9.2% globally and by 18.8% from East Asia. North American emissions decrease by 5.7%.

Impacts of electronically photo-excited NO<sub>2</sub> on air pollution in the South Coast Air Basin of California

Abstract. A new path for hydroxyl radical formation via photo-excitation of nitrogen dioxide (NO2) and the reaction of photo-excited NO2 with water is evaluated using the UCI-CIT model for the South Coast Air Basin of California (SoCAB). Two separate studies predict different reaction rates, which differ by nearly an order of magnitude, for the reaction of photo-excited NO2 with water. Impacts of this new chemical mechanism on ozone and particulate matter formation, while utilizing both reaction rates, are quantified by simulating two summer episodes. First, sensitivity simulations are conducted to evaluate the uncertainty in the rate of reaction of photo-excited NO2 with water reported in the literature. Results indicate that the addition of photo-excited NO2 chemistry increases peak 8-h average ozone and particulate matter concentrations. The importance of this new chemistry is then evaluated in the context of pollution control strategies. A series of simulations are conducted to generate isopleths for ozone and particulate matter concentrations, varying baseline nitrogen oxides (NOx) and volatile organic compounds (VOC) emissions. Isopleths are obtained using 1987 emissions, to represent past conditions, and 2005, to represent current conditions in the SoCAB. Results show that the sensitivity of modeled pollutant control strategies due to photoexcitation decreases with the decrease in baseline emissions from 1987 to 2005. Results show that including NO2 photo-excitation, increases the sensitivity of ozone concentration with respect to changes in NOx emissions for both years. In particular, decreasing NOx emissions in 2005 when NO2 photo-excitation is included, while utilizing the higher reaction rate, leads to ozone relative reduction factors that are 15% lower than in a case without photo-excited NO2. This implies that photoexcitation increases the effectiveness in reducing ozone through NOx emissions reductions alone, which has implications for the assessment of future emission control strategies. However, there is still disagreement with respect to the reaction rate constant for the formation of OH. Therefore, further studies are required to reduce the uncertainty in the reaction rate constant before this new mechanism is fully implemented in regulatory applications.

Evaluation of the use of photochemical indicators to assess ozone—NOx—VOC sensitivity in the Southwestern Iberian Peninsula

Understanding the chemical links between ozone (O3) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O3/NOy and O3/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.