scholarly journals Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

2012 ◽  
Vol 12 (9) ◽  
pp. 24243-24285 ◽  
Author(s):  
Y. Wang ◽  
Q. Q. Zhang ◽  
K. He ◽  
Q. Zhang ◽  
L. Chai
Keyword(s):  
Emission Reduction ◽  
Transport Model ◽  
Critical Role ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
So2 Emission ◽  
Dominant Component ◽  
Emission Changes ◽  
Emission Reduction Target

Abstract. We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA) aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3) from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60%~80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC) and Sichuan Basin (SCB), while nitrate makes equal contribution as sulfate over North China (NC). Based on emission reduction targets in the 12th (2011–2015) Five Year Plan (FYP), China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. However, the amount of NH3 emissions in 2015 is uncertain, given our finding that bottom-up inventories tend to overestimate China's ammonia emissions during the 2000–2006 period. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their levels in 2006, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

scholarly journals Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

2013 ◽  
Vol 13 (5) ◽  
pp. 2635-2652 ◽  
Author(s):  
Y. Wang ◽  
Q. Q. Zhang ◽  
K. He ◽  
Q. Zhang ◽  
L. Chai
Keyword(s):  
Emission Reduction ◽  
Transport Model ◽  
Critical Role ◽  
Sufficient Information ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Dominant Component ◽  
Emission Changes ◽  
Emission Reduction Target

Abstract. We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA) aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3) from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC) and Sichuan Basin (SCB), while nitrate and sulfate contribute equally over North China (NC). Based on emission reduction targets in the 12th (2011–2015) Five-Year Plan (FYP), China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

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

2014 ◽  
Vol 14 (3) ◽  
pp. 3427-3458
Author(s):  
C. D. Holmes ◽  
M. J. Prather ◽  
G. C. M. Vinken
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Parametric Representation ◽  
Climate Impact ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Rf Components ◽  
Maritime Shipping ◽  
Sensitivity Tests ◽  
Emission Changes

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 given in the past literature: +3.4 ± 0.85 mW m−2 from the short-lived ozone increase, −5.0 ± 1.1 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 −3.3 ± 1.8 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%).

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

2014 ◽  
Vol 14 (13) ◽  
pp. 6801-6812 ◽  
Author(s):  
C. D. Holmes ◽  
M. J. Prather ◽  
G. C. M. Vinken
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Parametric Representation ◽  
Climate Impact ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Rf Components ◽  
Maritime Shipping ◽  
Sensitivity Tests ◽  
Emission Changes

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%).

scholarly journals Assimilation of satellite NO<sub>2</sub> observations at high spatial resolution using OSSEs

2017 ◽  
Vol 17 (11) ◽  
pp. 7067-7081 ◽  
Author(s):  
Xueling Liu ◽  
Arthur P. Mizzi ◽  
Jeffrey L. Anderson ◽  
Inez Y. Fung ◽  
Ronald C. Cohen
Keyword(s):  
Data Assimilation ◽  
Transport Model ◽  
Weather Forecast ◽  
Forecast Errors ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Model Framework ◽  
Simulation Experiments ◽  
High Space

Abstract. Observations of trace gases from space-based instruments offer the opportunity to constrain chemical and weather forecast and reanalysis models using the tools of data assimilation. In this study, observing system simulation experiments (OSSEs) are performed to investigate the potential of high space- and time-resolution column measurements as constraints on urban NOx emissions. The regional chemistry–meteorology assimilation system where meteorology and chemical variables are simultaneously assimilated is comprised of a chemical transport model, WRF-Chem, the Data Assimilation Research Testbed, and a geostationary observation simulator. We design OSSEs to investigate the sensitivity of emission inversions to the accuracy and uncertainty of the wind analyses and the emission updating scheme. We describe the overall model framework and some initial experiments that point out the first steps toward an optimal configuration for improving our understanding of NOx emissions by combining space-based measurements and data assimilation. Among the findings we describe is the dependence of errors in the estimated NOx emissions on the wind forecast errors, showing that wind vectors with a RMSE below 1 m s−1 allow inference of NOx emissions with a RMSE of less than 30 mol/(km2  ×  h) at the 3 km scale of the model we use. We demonstrate that our inference of emissions is more accurate when we simultaneously update both NOx emissions and NOx concentrations instead of solely updating emissions. Furthermore, based on our analyses, we recommend carrying out meteorology assimilations to stabilize NO2 transport from the initial wind errors before starting the emission assimilation. We show that wind uncertainties (calculated as a spread around a mean wind) are not important for estimating NOx emissions when the wind uncertainties are reduced below 1.5 m s−1. Finally, we present results assessing the role of separate vs. simultaneous chemical and meteorological assimilation in a model framework without covariance between the meteorology and chemistry.

scholarly journals A new diagnostic for tropospheric ozone production

2017 ◽  
Author(s):  
Peter M. Edwards ◽  
Mathew J. Evans
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
Chemical Transport Model ◽  
Organic Species ◽  
Earth’S Climate ◽  
Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

Variability of PM pollution in the light of emission changes and meteorological variability: a case study for Styria, Austria

2020 ◽  
Author(s):  
Christian A. Schmidt ◽  
Peter Huszár ◽  
Monika Mayer ◽  
Johannes Fritzer ◽  
Harald E. Rieder
Keyword(s):  
Air Pollution ◽  
Emission Reduction ◽  
Transport Model ◽  
Special Importance ◽  
Chemistry Transport Model ◽  
The Alps ◽  
Industrial Regions ◽  
Emission Changes ◽  
Local Emissions

&lt;p&gt;Despite ambitious efforts to abate surface air pollution, the air quality thresholds for PM10 and PM2.5 are regularly exceeded in the state of Styria. PM target levels are most frequently exceeded in industrial regions and urban cores of the forelands preceeding the alps. Besides local emissions, ambient meteorology and particularly stagnation are of special importance for PM pollution. Here we assess local and regional changes in PM pollution following emission reduction measures, while simultaneously considering effects of meteorological variability. We further supplement our observational study with a set of high-resolution chemistry-transport-model (CTM) simulations to assess future changes in the PM burden in Styria.&lt;/p&gt;

scholarly journals Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC<sup>4</sup>RS) and ground-based (SOAS) observations in the Southeast US

2016 ◽  
Vol 16 (9) ◽  
pp. 5969-5991 ◽  
Author(s):  
Jenny A. Fisher ◽  
Daniel J. Jacob ◽  
Katherine R. Travis ◽  
Patrick S. Kim ◽  
Eloise A. Marais ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Transport Model ◽  
Oxidation Mechanism ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Particle Phase ◽  
Chemical Transport Model ◽  
Southeast Us

Abstract. Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with  ∼  25  ×  25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25–50 % of observed RONO2 in surface air, and we find that another 10 % is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10 % of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60 % of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20 % by photolysis to recycle NOx and 15 % by dry deposition. RONO2 production accounts for 20 % of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.

scholarly journals Long-term observational constraints of organic aerosol dependence on inorganic species in the southeast US

2020 ◽  
Author(s):  
Yiqi Zheng ◽  
Joel A. Thornton ◽  
Nga Lee Ng ◽  
Hansen Cao ◽  
Daven K. Henze ◽  
...  
Keyword(s):  
Air Quality ◽  
Transport Model ◽  
Organic Aerosol ◽  
Chemical Transport Model ◽  
Anthropogenic Pollutants ◽  
Aerosol Acidity ◽  
Inorganic Species ◽  
Southeast Us

Abstract. Organic aerosol (OA), with a large biogenic fraction in summertime southeast US, adversely impacts on air quality and human health. Stringent air quality controls have recently reduced anthropogenic pollutants including sulfate, whose impact on OA remains unclear. Three filter measurement networks provide long-term constraints on the sensitivity of OA to changes in inorganic species, including sulfate and ammonia. The 2000–2013 summertime OA decreases by 1.7~1.9 %/year with little month-to-month variability, while sulfate declines rapidly with significant monthly difference in early 2000s. In contrast, modeled OA from a chemical-transport model (GEOS-Chem) decreases by 4.9 %/year with much larger month-to-month variability, largely due to the predominant role of acid-catalyzed reactive uptake of epoxydiols (IEPOX) onto sulfate. The overestimated modeled OA dependence on sulfate can be improved by implementing a coating effect and assuming constant aerosol acidity, suggesting the needs to revisit IEPOX reactive uptake in current models. Our work highlights the importance of secondary OA formation pathways that are weakly dependent on inorganic aerosol in a region that is heavily influenced by both biogenic and anthropogenic emissions.

scholarly journals Global NO<sub>x</sub> emission estimates derived from an assimilation of OMI tropospheric NO<sub>2</sub> columns

2011 ◽  
Vol 11 (12) ◽  
pp. 31523-31583 ◽  
Author(s):  
K. Miyazaki ◽  
H. J. Eskes ◽  
K. Sudo
Keyword(s):  
Data Assimilation ◽  
Transport Model ◽  
A Priori ◽  
Eastern China ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Background Error ◽  
Tropospheric No2 ◽  
Data Assimilation System ◽  
Assimilation System

Abstract. A data assimilation system has been developed to estimate global nitrogen oxides (NOx) emissions using OMI tropospheric NO2 columns (DOMINO product) and a global chemical transport model (CTM), CHASER. The data assimilation system, based on an ensemble Kalman filter approach, was applied to optimize daily NOx emissions with a horizontal resolution of 2.8° during the years 2005 and 2006. The background error covariance estimated from the ensemble CTM forecasts explicitly represents non-direct relationships between the emissions and tropospheric columns caused by atmospheric transport and chemical processes. In comparison to the a priori emissions based on bottom-up inventories, the optimized emissions were higher over Eastern China, the Eastern United States, Southern Africa, and Central-Western Europe, suggesting that the anthropogenic emissions are mostly underestimated in the inventories. In addition, the seasonality of the estimated emissions differed from that of the a priori emission over several biomass burning regions, with a large increase over Southeast Asia in April and over South America in October. The data assimilation results were validated against independent data: SCIAMACHY tropospheric NO2 columns and vertical NO2 profiles obtained from aircraft and lidar measurements. The emission correction greatly improved the agreement between the simulated and observed NO2 fields; this implies that the data assimilation system efficiently derives NOx emissions from concentration observations. We also demonstrated that biases in the satellite retrieval and model settings used in the data assimilation largely affect the magnitude of estimated emissions. These dependences should be carefully considered for better understanding NOx sources from top-down approaches.

scholarly journals Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI

2021 ◽  
Vol 21 (24) ◽  
pp. 18227-18245
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Model Simulation ◽  
Surface Ozone ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Voc Emissions ◽  
Constrained Model

Abstract. Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. Accordingly, we jointly constrain NOx and VOC emissions using well-characterized TROPOspheric Monitoring Instrument (TROPOMI) HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NOx emissions in March 2020 (14 %–31 %) in several major cities including Paris, London, Madrid, and Milan, expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34 %–51 %) in April. However, NOx emissions remain at somewhat similar values or even higher in some portions of the UK, Poland, and Moscow in March 2020 compared to the baseline, possibly due to the timeline of restrictions. Comparisons against surface monitoring stations indicate that the constrained model underrepresents the reduction in surface NO2. This underrepresentation correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO2 reductions occurring in polluted areas are described fairly well by the model (model: −21 ± 17 %, observation: −29 ± 21 %). The observational constraint on VOC emissions is found to be generally weak except for lower latitudes. Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r=0.43), specifically over central Europe where ozone enhancements prevail (model: +3.73 ± 3.94 %, +1.79 ppbv, observation: +7.35 ± 11.27 %, +3.76 ppbv). The model suggests that physical processes (dry deposition, advection, and diffusion) decrease MDA8 surface ozone in the same month on average by −4.83 ppbv, while ozone production rates dampened by largely negative JNO2[NO2]-kNO+O3[NO][O3] become less negative, leading ozone to increase by +5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture ozone changes induced by abrupt emission anomalies.

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