scholarly journals Effects of temperature-dependent NO<sub>x</sub> emissions on continental ozone production

2017 ◽  
Author(s):  
Paul S. Romer ◽  
Kaitlin C. Duffey ◽  
Paul J. Wooldridge ◽  
Eric Edgerton ◽  
Karsten Baumann ◽  
...  

Abstract. Surface ozone concentrations are observed to increase with rising temperatures, but the mechanisms responsible for this effect in rural and remote continental regions remain uncertain. Better understanding of the effects of temperature on ozone is crucial to understanding global air quality and how it may be affected by climate change. We combine measurements from a focused ground campaign in summer 2013 with a long-term record from a forested site in the rural southeast United States to examine how daily average temperature affects ozone production. We find that changes to local chemistry are key drivers of increased ozone concentrations on hotter days, with integrated daily ozone production increasing by 2.3 ppb C−1. Nearly half of this increase is attributable to temperature-driven increases in emissions of nitrogen oxides (NOx), most likely by soil microbes. The increase of soil NOx emissions with temperature suggests that ozone will continue to increase with temperature in the future, even as direct anthropogenic NOx emissions decrease dramatically. The links between temperature, soil NOx, and ozone form a positive climate feedback.

2018 ◽  
Vol 18 (4) ◽  
pp. 2601-2614 ◽  
Author(s):  
Paul S. Romer ◽  
Kaitlin C. Duffey ◽  
Paul J. Wooldridge ◽  
Eric Edgerton ◽  
Karsten Baumann ◽  
...  

Abstract. Surface ozone concentrations are observed to increase with rising temperatures, but the mechanisms responsible for this effect in rural and remote continental regions remain uncertain. Better understanding of the effects of temperature on ozone is crucial to understanding global air quality and how it may be affected by climate change. We combine measurements from a focused ground campaign in summer 2013 with a long-term record from a forested site in the rural southeastern United States, to examine how daily average temperature affects ozone production. We find that changes to local chemistry are key drivers of increased ozone concentrations on hotter days, with integrated daily ozone production increasing by 2.3 ppb ∘C−1. Nearly half of this increase is attributable to temperature-driven increases in emissions of nitrogen oxides (NOx), most likely by soil microbes. The increase of soil NOx emissions with temperature suggests that ozone will continue to increase with temperature in the future, even as direct anthropogenic NOx emissions decrease dramatically. The links between temperature, soil NOx, and ozone form a positive climate feedback.


2021 ◽  
Author(s):  
Carla Gama ◽  
Alexandra Monteiro ◽  
Myriam Lopes ◽  
Ana Isabel Miranda

&lt;p&gt;Tropospheric ozone (O&lt;sub&gt;3&lt;/sub&gt;) is a critical pollutant over the Mediterranean countries, including Portugal, due to systematic exceedances to the thresholds for the protection of human health. Due to the location of Portugal, on the Atlantic coast at the south-west point of Europe, the observed O&lt;sub&gt;3&lt;/sub&gt; concentrations are very much influenced not only by local and regional production but also by northern mid-latitudes background concentrations. Ozone trends in the Iberian Peninsula were previously analysed by Monteiro et al. (2012), based on 10-years of O&lt;sub&gt;3&lt;/sub&gt; observations. Nevertheless, only two of the eleven background monitoring stations analysed in that study are located in Portugal and these two stations are located in Porto and Lisbon urban areas. Although during pollution events O&lt;sub&gt;3&lt;/sub&gt; levels in urban areas may be high enough to affect human health, the highest concentrations are found in rural locations downwind from the urban and industrialized areas, rather than in cities. This happens because close to the sources (e.g., in urban areas) freshly emitted NO locally scavenges O&lt;sub&gt;3&lt;/sub&gt;. A long-term study of the spatial and temporal variability and trends of the ozone concentrations over Portugal is missing, aiming to answer the following questions:&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; What is the temporal variability of ozone concentrations?&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; Which trends can we find in observations?&lt;/p&gt;&lt;p&gt;-&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; How were the ozone spring maxima concentrations affected by the COVID-19 lockdown during spring 2020?&lt;/p&gt;&lt;p&gt;In this presentation, these questions will be answered based on the statistical analysis of O&lt;sub&gt;3&lt;/sub&gt; concentrations recorded within the national air quality monitoring network between 2005 and 2020 (16 years). The variability of the surface ozone concentrations over Portugal, on the timescales from diurnal to annual, will be presented and discussed, taking into account the physical and chemical processes that control that variability. Using the TheilSen function from the OpenAir package for R (Carslaw and Ropkins 2012), which quantifies monotonic trends and calculates the associated p-value through bootstrap simulations, O&lt;sub&gt;3&lt;/sub&gt; concentration long-term trends will be estimated for the different regions and environments (e.g., rural, urban).&amp;#160; Moreover, taking advantage of the unique situation provided by the COVID-19 lockdown during spring 2020, when the government imposed mandatory confinement and citizens movement restriction, leading to a reduction in traffic-related atmospheric emissions, the role of these emissions on ozone levels during the spring period will be studied and presented.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Carslaw and Ropkins, 2012. Openair&amp;#8212;an R package for air quality data analysis. Environ. Model. Softw. 27-28,52-61. https://doi.org/10.1016/j.envsoft.2011.09.008&lt;/p&gt;&lt;p&gt;Monteiro et al., 2012. Trends in ozone concentrations in the Iberian Peninsula by quantile regression and clustering. Atmos. Environ. 56, 184-193. https://doi.org/10.1016/j.atmosenv.2012.03.069&lt;/p&gt;


2016 ◽  
Vol 16 (18) ◽  
pp. 11601-11615 ◽  
Author(s):  
Jane Coates ◽  
Kathleen A. Mar ◽  
Narendra Ojha ◽  
Tim M. Butler

Abstract. Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NOx). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NOx and temperature, and we compared this to previous observational studies. Under high-NOx conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NOx emissions. CB05 and RADM2 simulated more NOx-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of Ox production; the net influence of peroxy nitrates increased net Ox production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NOx emissions would be required to offset the additional ozone production due to an increase in temperature in the future.


2010 ◽  
Vol 10 (14) ◽  
pp. 6645-6660 ◽  
Author(s):  
P. Huszar ◽  
D. Cariolle ◽  
R. Paoli ◽  
T. Halenka ◽  
M. Belda ◽  
...  

Abstract. In general, regional and global chemistry transport models apply instantaneous mixing of emissions into the model's finest resolved scale. In case of a concentrated source, this could result in erroneous calculation of the evolution of both primary and secondary chemical species. Several studies discussed this issue in connection with emissions from ships and aircraft. In this study, we present an approach to deal with the non-linear effects during dispersion of NOx emissions from ships. It represents an adaptation of the original approach developed for aircraft NOx emissions, which uses an exhaust tracer to trace the amount of the emitted species in the plume and applies an effective reaction rate for the ozone production/destruction during the plume's dilution into the background air. In accordance with previous studies examining the impact of international shipping on the composition of the troposphere, we found that the contribution of ship induced surface NOx to the total reaches 90% over remote ocean and makes 10–30% near coastal regions. Due to ship emissions, surface ozone increases by up to 4–6 ppbv making 10% contribution to the surface ozone budget. When applying the ship plume parameterization, we show that the large scale NOx decreases and the ship NOx contribution is reduced by up to 20–25%. A similar decrease was found in the case of O3. The plume parameterization suppressed the ship induced ozone production by 15–30% over large areas of the studied region. To evaluate the presented parameterization, nitrogen monoxide measurements over the English Channel were compared with modeled values and it was found that after activating the parameterization the model accuracy increases.


2018 ◽  
Vol 18 (3) ◽  
pp. 2341-2361 ◽  
Author(s):  
Jingyi Li ◽  
Jingqiu Mao ◽  
Arlene M. Fiore ◽  
Ronald C. Cohen ◽  
John D. Crounse ◽  
...  

Abstract. Widespread efforts to abate ozone (O3) smog have significantly reduced emissions of nitrogen oxides (NOx) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NOx emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (July–August 2004), SENEX (June–July 2013), and SEAC4RS (August–September 2013) and long-term ground measurement networks alongside a global chemistry–climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NOy) in both 2004 and 2013. Among the major RON species, nitric acid (HNO3) is dominant (∼ 42–45 %), followed by NOx (31 %), total peroxy nitrates (ΣPNs; 14 %), and total alkyl nitrates (ΣANs; 9–12 %) on a regional scale. We find that most RON species, including NOx, ΣPNs, and HNO3, decline proportionally with decreasing NOx emissions in this region, leading to a similar decline in NOy. This linear response might be in part due to the nearly constant summertime supply of biogenic VOC emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NOx emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.


2014 ◽  
Vol 14 (3) ◽  
pp. 1385-1396 ◽  
Author(s):  
H. Lei ◽  
J. X. L. Wang

Abstract. As precursors to tropospheric ozone and nitrate, nitrogen oxide (NOx) in the present atmosphere and its transformation in response to emission and climate perturbations are studied by using the CAM-Chem model and air quality measurements from the National Emissions Inventory (NEI), Clean Air Status and Trends Network (CASTNET), and Environmental Protection Agency Air Quality System (EPA AQS). It is found that NOx transformations in present atmospheric conditions show different sensitivities over industrial and non-industrial regions. As a result, the surface ozone and nitrate formations can be divided into several regimes associated with the dominant emission types and relative levels of NOx and volatile organic compounds (VOC). Ozone production in industrial regions (the main NOx emission source areas) increases in warmer conditions and slightly decreases following an increase in NOx emissions due to NOx titration, which is opposite to the response in non-industrial regions. The ozone decrease following a temperature increase in non-industrial regions indicates that ozone production in regions that lack NOx emission sources may be sensitive to NOx transformation in remote source regions. The increase in NO2 from NOx titration over industrial regions results in an increase rate of total nitrate that remains higher than the increase rate of NOx emissions. The presented findings indicate that a change in the ozone concentration is more directly affected by changes in climate and precursor emissions, while a change in the nitrate concentration is affected by local ozone production types and their seasonal transfer. The sensitivity to temperature perturbations shows that a warmer climate accelerates the decomposition of odd nitrogen (NOy) during the night. As a result, the transformation rate of NOx to nitrate decreases. Examinations of the historical emissions and air quality records of a typical NOx-limited area, such as Atlanta and a VOC-limited area, such as Los Angeles further confirm the conclusions drawn from the modeling experiments.


2010 ◽  
Vol 10 (8) ◽  
pp. 3827-3846 ◽  
Author(s):  
J. Song ◽  
W. Lei ◽  
N. Bei ◽  
M. Zavala ◽  
B. de Foy ◽  
...  

Abstract. The sensitivity of ozone production to precursor emissions was investigated under five different meteorological conditions in the Mexico City Metropolitan Area (MCMA) during the MCMA-2006/MILAGRO field campaign using the gridded photochemical model CAMx driven by observation-nudged WRF meteorology. Precursor emissions were constrained by the comprehensive data from the field campaign and the routine ambient air quality monitoring network. Simulated plume mixing and transport were examined by comparing with measurements from the G-1 aircraft during the campaign. The observed concentrations of ozone precursors and ozone were reasonably well reproduced by the model. The effects of reducing precursor emissions on urban ozone production were performed for three representative emission control scenarios. A 50% reduction in VOC emissions led to 7 to 22 ppb decrease in daily maximum ozone concentrations, while a 50% reduction in NOx emissions leads to 4 to 21 ppb increase, and 50% reductions in both NOx and VOC emission decrease the daily maximum ozone concentrations up to 10 ppb. These results along with a chemical indicator analysis using the chemical production ratios of H2O2 to HNO3 demonstrate that the MCMA urban core region is VOC-limited for all meteorological episodes, which is consistent with the results from MCMA-2003 field campaign; however the degree of the VOC-sensitivity is higher during MCMA-2006 due to lower VOCs, lower VOC reactivity and moderately higher NOx emissions. Ozone formation in the surrounding mountain/rural area is mostly NOx-limited, but can be VOC-limited, and the range of the NOx-limited or VOC-limited areas depends on meteorology.


2021 ◽  
Author(s):  
Zhenze Liu ◽  
Ruth M. Doherty ◽  
Oliver Wild ◽  
Fiona M. O’Connor ◽  
Steven T. Turnock

Abstract. Tropospheric ozone is important to future air quality and climate. We investigate ozone changes and ozone sensitivity to changing emissions in the context of climate change from the present day (2004–2014) to the future (2045–2055) under a range of shared socio-economic pathways (SSPs). We apply the United Kingdom Earth System Model, UKESM1, with an extended chemistry scheme including more reactive volatile organic compounds (VOCs) to quantify ozone burdens as well as ozone sensitivities globally and regionally based on nitrogen oxide (NOx) and VOC concentrations. We show that the tropospheric ozone burden increases by 4 % under a development pathway with higher NOx and VOC emissions (SSP3-7.0), but decreases by 7 % under the same pathway if NOx and VOC emissions are reduced (SSP3-7.0-lowNTCF) and by 5 % if atmospheric methane (CH4) concentrations are reduced (SSP3-7.0-lowCH4). Global mean surface ozone concentrations are reduced by 3–5 ppb under SSP3-7.0-lowNTCF and by 2–3 ppb under SSP3-7.0-lowCH4. However, surface ozone changes vary substantially by season in high-emission regions under future pathways, with decreased ozone concentrations in summer and increased ozone concentrations in winter when NOx emissions are reduced. VOC-limited areas are more extensive in winter (7 %) than in summer (3 %) across the globe. North America, Europe and East Asia are the dominant VOC-limited regions in the present day but North America and Europe become more NOx-limited in the future mainly due to reductions in NOx emissions. The impacts of VOC emissions on O3 sensitivity are limited in North America and Europe because reduced anthropogenic VOC emissions are offset by higher biogenic VOC emissions. O3 sensitivity is not greatly influenced by changing CH4 concentrations. South Asia becomes the dominant VOC-limited region under future pathways. We highlight that reductions in NOx emissions are required to transform O3 production from VOC- to NOx-limitation, but that these lead to increased O3 concentrations in high-emission regions, and hence emission controls on VOC and CH4 are also necessary.


2009 ◽  
Vol 9 (2) ◽  
pp. 7079-7113 ◽  
Author(s):  
J. J. West ◽  
V. Naik ◽  
L. W. Horowitz ◽  
A. M. Fiore

Abstract. Large-scale changes in ozone precursor emissions affect ozone directly in the short term, and also affect methane, which in turn causes long-term changes in ozone that affect surface ozone air quality. Here we assess the effects of changes in ozone precursor emissions on the long-term change in surface ozone via methane, as a function of the emission region, by modeling 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions. Reductions in NOx emissions from all world regions increase methane and long-term surface ozone. While this long-term increase is small compared to the intra-regional short-term ozone decrease, it is comparable to or larger than the short-term inter-continental ozone decrease for some source-receptor pairs. The increase in methane and long-term surface ozone per ton of NOx reduced is greatest in tropical and Southern Hemisphere regions, exceeding that from temperate Northern Hemisphere regions by roughly a factor of ten. We also assess changes in premature ozone-related human mortality associated with regional precursor reductions and long-range transport, showing that for 10% regional NOx reductions, the strongest inter-regional influence is for emissions from Europe affecting mortalities in Africa. Reductions of NOx in North America, Europe, the Former Soviet Union, and Australia are shown to reduce more mortalities outside of the source regions than within. Among world regions, NOx reductions in India cause the greatest number of avoided mortalities per ton, mainly in India itself. Finally, by increasing global methane, NOx reductions in one hemisphere tend to cause long-term increases in ozone concentration and mortalities in the opposite hemisphere. Reducing emissions of methane, and to a lesser extent carbon monoxide and non-methane volatile organic compounds, alongside NOx reductions would avoid this disbenefit.


2021 ◽  
Vol 21 (24) ◽  
pp. 18227-18245
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  

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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