scholarly journals Estimate of Secondary NO2 Levels at Two Urban Traffic Sites Using Observations and Modelling

2020 ◽  
Vol 12 (19) ◽  
pp. 7897 ◽  
Author(s):  
Grazia Ghermandi ◽  
Sara Fabbi ◽  
Giorgio Veratti ◽  
Alessandro Bigi ◽  
Sergio Teggi

Assessing secondary and primary NO2 in urban areas is important to support carefully designed environmental policies, particularly in areas with recurrent exceedance of NO2 regulatory limits. The share of secondary NO2 was preliminary estimated in intense traffic areas of Modena and Reggio Emilia (Northern Italy) by the combined analysis of regulatory air quality observations at urban traffic and urban background conditions. In addition simulations performed by the Lagrangian particle dispersion models Micro SWIFT SPRAY and the chemical transport model WRF-Chem were performed. The former was applied on the urban area representative of traffic conditions for both cities, in winter. The latter was applied twice in Modena, both with and without urban traffic emissions. Results suggest a large amount of secondary NO2 mainly at the Modena traffic site, and a better representativity of background conditions of the corresponding urban station in Reggio Emilia. NOx levels simulated by WRF-Chem show good results at Modena urban background and performance in line with reference benchmark values in reproducing observed NO2 and NOx concentrations at rural background sites, although a non-negligible bias in simulated urban NO2 remained. Overall the simulation models suggest that contribution to atmospheric NOx by domestic heating or industrial combustion emissions are not as relevant compared to traffic, consistently with the local emission inventory.

2016 ◽  
Author(s):  
Sam J. Silva ◽  
Colette L. Heald ◽  
Jeffrey A. Geddes ◽  
Kemen G. Austin ◽  
Prasad S. Kasibhatla ◽  
...  

Abstract. Over recent decades oil palm plantations have rapidly expanded across Southeast Asia (SEA). According to the United Nations, oil palm production in SEA increased by a factor of 3 from 1995 to 2010. We investigate the impacts of current (2010) and future (2020) oil palm expansion in SEA on surface-atmosphere exchange and the resulting air quality in the region. For this purpose, we use satellite data, high-resolution land maps, and the chemical transport model GEOS-Chem. Relative to a no oil palm plantation scenario (~ 1990), overall simulated isoprene emissions in the region increase by 13 % due to oil palm plantations in 2010 and a further 11 % by 2020. In addition, the expansion of palm plantations leads to local increases in ozone deposition velocities of up to 20 %. The net result of these changes is that oil palm expansion in SEA increases surface O3 by up to 3.5 ppbv over dense urban regions, and could rise more than 4.5 ppbv above baseline levels by 2020. Biogenic secondary organic aerosol loadings also increase by up to 1 μg m−3 due to oil palm expansion, and could increase a further 2.5 μg m−3 by 2020. Our analysis indicates that while the impact of recent oil palm expansion on air quality in the region has been significant, the retrieval error and sensitivity of the current constellation of satellite measurements limit our ability to observe these impacts from space. Oil palm expansion is likely to continue to degrade air quality in the region in the coming decade and hinder efforts to achieve air quality regulations in major urban areas such as Kuala Lumpur and Singapore.


2011 ◽  
Vol 11 (18) ◽  
pp. 9887-9898 ◽  
Author(s):  
M. Rigby ◽  
A. J. Manning ◽  
R. G. Prinn

Abstract. We present a method for estimating emissions of long-lived trace gases from a sparse global network of high-frequency observatories, using both a global Eulerian chemical transport model and Lagrangian particle dispersion model. Emissions are derived in a single step after determining sensitivities of the observations to initial conditions, the high-resolution emissions field close to observation points, and larger regions further from the measurements. This method has the several advantages over inversions using one type of model alone, in that: high-resolution simulations can be carried out in limited domains close to the measurement sites, with lower resolution being used further from them; the influence of errors due to aggregation of emissions close to the measurement sites can be minimized; assumptions about boundary conditions to the Lagrangian model do not need to be made, since the entire emissions field is estimated; any combination of appropriate models can be used, with no code modification. Because the sensitivity to the entire emissions field is derived, the estimation can be carried out using traditional statistical methods without the need for multiple steps in the inversion. We demonstrate the utility of this approach by determining global SF6 emissions using measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) between 2007 and 2009. The global total and large-scale patterns of the derived emissions agree well with previous studies, whilst allowing emissions to be determined at higher resolution than has previously been possible, and improving the agreement between the modeled and observed mole fractions at some sites.


2017 ◽  
Vol 17 (14) ◽  
pp. 8757-8770 ◽  
Author(s):  
Roghayeh Ghahremaninezhad ◽  
Ann-Lise Norman ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  

Abstract. Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster Sound, Nunavut, Canada, in July 2014 and on pan-Arctic flights in April 2015 that started from Longyearbyen, Spitzbergen, and passed through Alert and Eureka, Nunavut, and Inuvik, Northwest Territories. Larger mean DMS(g) mixing ratios were present during April 2015 (campaign mean of 116  ±  8 pptv) compared to July 2014 (campaign mean of 20  ±  6 pptv). During July 2014, the largest mixing ratios were found near the surface over the ice edge and open water. DMS(g) mixing ratios decreased with altitude up to about 3 km. During April 2015, profiles of DMS(g) were more uniform with height and some profiles showed an increase with altitude. DMS reached as high as 100 pptv near 2500 m. Relative to the observation averages, GEOS-Chem (www.geos-chem.org) chemical transport model simulations were higher during July and lower during April. Based on the simulations, more than 90 % of the July DMS(g) below 2 km and more than 90 % of the April DMS(g) originated from Arctic seawater (north of 66° N). During April, 60 % of the DMS(g), between 500 and 3000 m originated from Arctic seawater. During July 2014, FLEXPART (FLEXible PARTicle dispersion model) simulations locate the sampled air mass over Baffin Bay and the Canadian Arctic Archipelago 4 days back from the observations. During April 2015, the locations of the air masses 4 days back from sampling were varied: Baffin Bay/Canadian Archipelago, the Arctic Ocean, Greenland and the Pacific Ocean. Our results highlight the role of open water below the flight as the source of DMS(g) during July 2014 and the influence of long-range transport (LRT) of DMS(g) from further afield in the Arctic above 2500 m during April 2015.


2009 ◽  
Vol 2 (1) ◽  
pp. 185-207 ◽  
Author(s):  
P. Eller ◽  
K. Singh ◽  
A. Sandu ◽  
K. Bowman ◽  
D. K. Henze ◽  
...  

Abstract. This paper discusses the implementation and performance of an array of gas-phase chemistry solvers for the state-of-the-science GEOS-Chem global chemical transport model. The implementation is based on the Kinetic PreProcessor (KPP). Two perl parsers automatically generate the needed interfaces between GEOS-Chem and KPP, and allow access to the chemical simulation code without any additional programming effort. This work illustrates the potential of KPP to positively impact global chemical transport modeling by providing additional functionality as follows. (1) The user can select a highly efficient numerical integration method from an array of solvers available in the KPP library. (2) KPP offers extreme flexibility for studies that involve changing the chemical mechanism (e.g., a set of additional reactions is automatically translated into efficient code and incorporated into a modified global model). (3) This work provides immediate access to tangent linear, continuous adjoint, and discrete adjoint chemical models, with applications to sensitivity analysis and data assimilation.


2012 ◽  
Vol 12 (4) ◽  
pp. 8771-8822 ◽  
Author(s):  
A. G. Megaritis ◽  
C. Fountoukis ◽  
P. E. Charalampidis ◽  
C. Pilinis ◽  
S. N. Pandis

Abstract. PMCAMx-2008, a three dimensional chemical transport model (CTM), was applied in Europe to quantify the changes in fine particle (PM2.5) concentration in response to different emission reductions as well as to temperature increase. A summer and a winter simulation period were used, to investigate the seasonal dependence of the PM2.5 response to 50% reductions of SO2, NH3, NOx, anthropogenic VOCs and anthropogenic OA emissions and also to temperature increases of 2.5 and 5 K. Reduction of NH3 emissions seems to be the most effective control strategy for reducing PM2.5, in both periods, resulting in a decrease of PM2.5 up to 5.1 μg m−3 and 1.8 μg m−3 (5.5% and 4% on average) during summer and winter respectively, mainly due to reduction of NH4NO3 (20% on average in both periods). The reduction of SO2 emissions decreases PM2.5 in both periods having a significant effect over the Balkans (up to 1.6 μg m−3) during summer, mainly due to decrease of sulfate (30% on average over the Balkans). The anthropogenic OA control strategy reduces total OA by 15% during winter and 8% in the summer. The reduction of total OA is higher in urban areas close to its emissions sources. A slight decrease of OA (8% in summer and 4% in winter) is also predicted after a 50% reduction of VOCs emissions due to the decrease of anthropogenic SOA. The reduction of NOx emissions reduces PM2.5 (up to 3.4 μg m−3) during the summer, due a decrease of NH4NO3, causing although an increase of ozone concentration in major urban areas and over Western Europe. Additionally, the NOx control strategy actually increases PM2.5 levels during the winter. The increase of temperature results in a decrease of PM2.5 in both periods over Central Europe, mainly due to a decrease of NH4NO3 during summer (18%) and fresh POA during winter (35%). Significant increases of OA are usually predicted during summer due mainly to the increase of biogenic VOC emissions. On the contrary, OA is predicted to decrease in the winter due to the dominance of fresh POA reduction and the small biogenic SOA contribution to OA. The resulting increase of oxidant levels from the temperature rise lead to an increase of sulfate levels in both periods, mainly over North Europe and the Atlantic Ocean. The substantial reduction of PM2.5 components due to emissions reductions of their precursors in conjunction with significant changes of PM after increasing the temperature indicate that both emissions and temperature need to be of significant concern for improving air quality.


2011 ◽  
Vol 11 (11) ◽  
pp. 5153-5168 ◽  
Author(s):  
A. P. Tsimpidi ◽  
V. A. Karydis ◽  
M. Zavala ◽  
W. Lei ◽  
N. Bei ◽  
...  

Abstract. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 includes the recently developed volatility basis-set framework in which both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico de Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites is encouraging. The average predicted PM1 organic aerosol (OA) concentration in T0, T1, and T2 is 18 μg m−3, 11.7 μg m−3, and 10.5 μg m−3 respectively, while the corresponding measured values are 17.2 μg m−3, 11 μg m−3, and 9 μg m−3. The average predicted locally-emitted primary OA concentrations, 4.4 μg m−3 at T0, 1.2 μg m−3 at T1 and 1.7 μg m−3 at PTP, are in reasonably good agreement with the corresponding PMF analysis estimates based on the Aerosol Mass Spectrometer (AMS) observations of 4.5, 1.3, and 2.9 μg m−3 respectively. The model reproduces reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m−3 predicted versus 7.5 μg m−3 measured), in T1 (6.3 μg m−3 predicted versus 4.6 μg m−3 measured) and in PTP (6.6 μg m−3 predicted versus 5.9 μg m−3 measured). The rest of the OA mass (6.1 μg m−3 and 4.2 μg m−3 in T0 and T1 respectively) is assumed to originate from biomass burning activities and is introduced to the model as part of the boundary conditions. Inside Mexico City (at T0), the locally-produced OA is predicted to be on average 60 % locally-emitted primary (POA), 6 % semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 34 % traditional SOA from the oxidation of VOCs (V-SOA). The average contributions of the OA components to the locally-produced OA for the entire modelling domain are predicted to be 32 % POA, 10 % S-SOA and I-SOA, and 58 % V-SOA. The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period.


2018 ◽  
Vol 18 (11) ◽  
pp. 7799-7814 ◽  
Author(s):  
Jia Xing ◽  
Dian Ding ◽  
Shuxiao Wang ◽  
Bin Zhao ◽  
Carey Jang ◽  
...  

Abstract. As one common precursor for both PM2.5 and O3 pollution, NOx gains great attention because its controls can be beneficial for reducing both PM2.5 and O3. However, the effectiveness of NOx controls for reducing PM2.5 and O3 are largely influenced by the ambient levels of NH3 and VOC, exhibiting strong nonlinearities characterized as NH3-limited/NH3-poor and NOx-/VOC-limited conditions, respectively. Quantification of such nonlinearities is a prerequisite for making suitable policy decisions but limitations of existing methods were recognized. In this study, a new method was developed by fitting multiple simulations of a chemical transport model (i.e., Community Multiscale Air Quality Modeling System, CMAQ) with a set of polynomial functions (denoted as “pf-RSM”) to quantify responses of ambient PM2.5 and O3 concentrations to changes in precursor emissions. The accuracy of the pf-RSM is carefully examined to meet the criteria of a mean normalized error within 2 % and a maximal normalized error within 10 % by using 40 training samples with marginal processing. An advantage of the pf-RSM method is that the nonlinearity in PM2.5 and O3 responses to precursor emission changes can be characterized by quantitative indicators, including (1) a peak ratio (denoted as PR) representing VOC-limited or NOx-limited conditions, (2) a suggested ratio of VOC reduction to NOx reduction to avoid increasing O3 under VOC-limited conditions, (3) a flex ratio (denoted as FR) representing NH3-poor or NH3-rich conditions, and (4) enhanced benefits in PM2.5 reductions from simultaneous reduction of NH3 with the same reduction rate of NOx. A case study in the Beijing–Tianjin–Hebei region suggested that most urban areas present strong VOC-limited conditions with a PR from 0.4 to 0.8 in July, implying that the NOx emission reduction rate needs to be greater than 20–60 % to pass the transition from VOC-limited to NOx-limited conditions. A simultaneous VOC control (the ratio of VOC reduction to NOx reduction is about 0.5–1.2) can avoid increasing O3 during the transition. For PM2.5, most urban areas present strong NH3-rich conditions with a PR from 0.75 to 0.95, implying that NH3 is sufficiently abundant to neutralize extra nitric acid produced by an additional 5–35 % of NOx emissions. Enhanced benefits in PM2.5 reductions from simultaneous reduction of NH3 were estimated to be 0.04–0.15 µg m−3 PM2.5 per 1 % reduction of NH3 along with NOx, with greater benefits in July when the NH3-rich conditions are not as strong as in January. Thus, the newly developed pf-RSM model has successfully quantified the enhanced effectiveness of NOx control, and simultaneous reduction of VOC and NH3 with NOx can assure the control effectiveness of PM2.5 and O3.


2009 ◽  
Vol 6 (3) ◽  
pp. 219 ◽  
Author(s):  
Timothy M. Butler ◽  
Mark G. Lawrence

Environmental context. Over half of the population of the world now live in urban areas, and the number of so-called ‘megacities’, with populations of ~10 million or more, is growing at a tremendous rate. We show how these patterns of urbanisation have the potential to influence the atmospheric chemical environment on a global scale, particularly through the effects of emissions from megacities on the reactive nitrogen cycle. With the growing worldwide interest in the study of the effects of megacities at all spatial scales, such as current European Union projects MEGAPOLI and CityZen, our study represents the first of many future studies that examine the effects of megacities on atmospheric chemistry on the global scale. Abstract. We present the first study of the effects of megacities on global atmospheric chemistry using a global three-dimensional chemical transport model. The effects on air quality, radiative forcing and atmospheric oxidation capacity are disproportionately smaller than the proportion of anthropogenic emissions due to megacities. Disproportionately large effects of megacities are modelled for reactive nitrogen compounds, in particular PAN (peroxy acetyl nitrate), which has increased in abundance globally by 9% due to megacities under year 2000 conditions, with 23% of the Earth experiencing an increase of 10% or more. These influences decrease under two very different future emission scenarios. Under a low-emission future scenario, the influence of megacities is generally reduced, and under a high-emission future scenario, although the local influence of megacities is increased, the geographical extent of the influence becomes smaller. In our model, the individual grid cells that contain megacities respond to the megacity emissions differently depending on their latitude. Tropical megacity grid cells generally show increased ozone year-round, while northern extratropical megacities generally show reduced ozone year-round. Better parameterisation of the sub-grid effects of megacities is an important issue for future work.


2019 ◽  
Vol 5 (4) ◽  
pp. eaav4707 ◽  
Author(s):  
Delin Fang ◽  
Bin Chen ◽  
Klaus Hubacek ◽  
Ruijing Ni ◽  
Lulu Chen ◽  
...  

China has enacted a number of ambitious pollution control policies to mitigate air pollution in urban areas. Unintended side effects of these policies to other environmental policy arenas and regions have largely been ignored. To bridge this gap, we use a multiregional input-output model in combination with an atmospheric chemical transport model to simulate clean air policy scenarios and evaluate their environmental impacts on primary PM2.5and secondary precursor emissions, as well as CO2emissions and water consumption, in the target region and spillover effects to other regions. Our results show that the reduction in primary PM2.5and secondary precursor emissions in the target regions comes at the cost of increasing emissions especially in neighboring provinces. Similarly, co-benefits of lower CO2emissions and reduced water consumption in the target region are achieved at the expense of higher impacts elsewhere, through outsourcing production to less developed regions in China.


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