scholarly journals Ozone Response to Emission Reductions in the Southeastern United States

Author(s):  
Charles L. Blanchard ◽  
George M. Hidy

Abstract. Ozone (O3) formation in the southeastern U.S. is studied in relation to nitrogen oxide (NOx) emissions using long-term (1990s–2015) surface measurements of the Southeastern Aerosol Research and Characterization (SEARCH) network, U.S. Environmental Protection Agency (EPA) O3 measurements, and EPA Clean Air Status and Trends Network (CASTNet) nitrate deposition data. CASTNet data show declining wet and dry nitrate deposition since the late 1990s, with total (wet plus dry) nitrate deposition fluxes decreasing linearly in proportion to reductions of NOx emissions in in Alabama and Georgia. Annual nitrate deposition rates at Georgia and Alabama CastNet sites correspond to 30 % of Georgia emission rates and 36 % of Alabama emission rates, respectively. The fraction of NOx emissions lost to deposition has not changed over time. SEARCH and EPA CASTNet sites exhibit comparable downward trends in mean annual nitric acid (HNO3) concentrations. Mean annual total oxidized nitrogen (NOy) mixing ratios at SEARCH sites declined in proportion to NOx emission reductions. Annual 4th-highest daily peak 8-hour O3 mixing ratios at EPA monitoring sites in Georgia, Alabama, and Mississippi exhibit statistically-significant (p 

2018 ◽  
Vol 18 (11) ◽  
pp. 8183-8202 ◽  
Author(s):  
Charles L. Blanchard ◽  
George M. Hidy

Abstract. Ozone (O3) formation in the southeastern US is studied in relation to nitrogen oxide (NOx) emissions using long-term (1990s–2015) surface measurements of the Southeastern Aerosol Research and Characterization (SEARCH) network, U.S. Environmental Protection Agency (EPA) O3 measurements, and EPA Clean Air Status and Trends Network (CASTNET) nitrate deposition data. Annual fourth-highest daily peak 8 h O3 mixing ratios at EPA monitoring sites in Georgia, Alabama, and Mississippi exhibit statistically significant (p < 0.0001) linear correlations with annual NOx emissions in those states between 1996 and 2015. The annual fourth-highest daily peak 8 h O3 mixing ratios declined toward values of ∼ 45–50 ppbv and monthly O3 maxima decreased at rates averaging ∼ 1–1.5 ppbv yr−1. Mean annual total oxidized nitrogen (NOy) mixing ratios at SEARCH sites declined in proportion to NOx emission reductions. CASTNET data show declining wet and dry nitrate deposition since the late 1990s, with total (wet plus dry) nitrate deposition fluxes decreasing linearly in proportion to reductions of NOx emissions by ∼ 60 % in Alabama and Georgia. Annual nitrate deposition rates at Georgia and Alabama CASTNET sites correspond to 30 % of Georgia emission rates and 36 % of Alabama emission rates, respectively. The fraction of NOx emissions lost to deposition has not changed. SEARCH and CASTNET sites exhibit downward trends in mean annual nitric acid (HNO3) concentrations. Observed relationships of O3 to NOz (NOy–NOx) support past model predictions of increases in cycling of NO and increasing responsiveness of O3 to NOx. The study data provide a long-term record that can be used to examine the accuracy of process relationships embedded in modeling efforts. Quantifying observed O3 trends and relating them to reductions in ambient NOy species concentrations offers key insights into processes of general relevance to air quality management and provides important information supporting strategies for reducing O3 mixing ratios.


2020 ◽  
Author(s):  
Mengyao Liu ◽  
Ronald Van der A ◽  
Haiyue Tan ◽  
Christian Frankenberg ◽  
Ilse Aben ◽  
...  

&lt;p&gt;Methane (CH4) is the most important anthropogenic greenhouse gas after carbon dioxide, and it keeps increasing globally since 2007 after a period of relative stability, which is well-documented by surface measurements and satellites. Although satellites provide long-term global observations of CH4, the interpretation of column-averaged mixing ratios (xCH4) is difficult due to the influence of elevated terrains (i.e. mountain areas) and less abundant methane in the stratosphere. The lack of data over the ocean further limits global insights. Here we build a long-term global CH4 data set at a resolution of 0.25&amp;#176; &amp;#215; 0.25&amp;#176; &amp;#160;from SCIAMACHY, including the areas over the ocean, with the help of FRESCO cloud data. We dynamically consider the influence of elevations and contributions from the stratosphere through converting xCH4 to tropospheric xCH4 (trop_xCH4) by applying the daily ratios of tropospheric to stratospheric xCH4 in GEOS-Chem model.&lt;/p&gt;&lt;p&gt;The large increases occur in Trop_xCH4 over the source regions and mountain areas. The trend of SCIAMACHY Trop_xCH4 over the global ocean is comparable to the trend of NOAA globally averaged marine monthly mean data, showing the capability of SCIAMACHY in monitoring the ocean. After removing the latitudinally independent background concentration based on SCIAMACHY data over the ocean, we quantify the regional sources. A significant trend in Trop_ xCH4 relating to the background in Eastern China, India, tropical Africa, and tropical South America is further found from 2003 to 2011.&amp;#160;&lt;/p&gt;


2009 ◽  
Vol 9 (22) ◽  
pp. 9083-9099 ◽  
Author(s):  
L. M. O'Brien ◽  
N. R. P. Harris ◽  
A. D. Robinson ◽  
B. Gostlow ◽  
N. Warwick ◽  
...  

Abstract. A new gas chromatograph was used to make measurements of halocarbons at the Cape Verde observatory during late May and early June 2007. The instrument demonstrated its potential for long-term autonomous measurements. Bromoform (CHBr3) exhibits the most variability of all the halocarbons observed, ranging from a background concentration of about 4 ppt to a maximum of >40 ppt during the course of the measurement period. CH2Br2 correlates well with bromoform, suggesting a common regional source. Methyl iodide does not correlate with these bromocarbons, with base levels of around 1–2 ppt and some periods of much higher mixing ratios. Using published bromocarbon emission rates, our chemical transport model studies, presented here, do not reproduce the observations. Local emission magnitudes and CHBr3:CH2Br2 ratios must be increased more in line with the recent observations of Yokouchi et al. (2005) to improve the model to measurement comparison. Even when the model reproduces the observed bromocarbons, modelled BrO is much less than recent tropical observations (Read et al., 2008). A sea salt source seems the likely explanation. When high BrO is reproduced, the model agrees much better with the observed ozone changes, including diurnal variation, during the measurement period but it is suggested that a representation of iodine chemistry in the model is also required.


2009 ◽  
Vol 9 (1) ◽  
pp. 4335-4379 ◽  
Author(s):  
L. M. O'Brien ◽  
N. R. P. Harris ◽  
A. D. Robinson ◽  
B. Gostlow ◽  
N. Warwick ◽  
...  

Abstract. A new gas chromatograph was used to make measurements of halocarbons at the Cape Verde observatory during late May and early June 2007. The instrument demonstrated its potential for long-term autonomous measurements. Bromoform (CHBr3) exhibits the most variability of all the halocarbons observed, ranging from a background concentration of about 4 ppt to a maximum of >40 ppt during the course of the measurement period. Dibromomethane (CH2Br2) correlates well with CHBr3, suggesting a common regional source. Methyl iodide (CH3I) does not correlate with these bromocarbons, with base levels of around 1–2 ppt and some periods of much higher mixing ratios. Model studies with published bromocarbon emission rates do not reproduce the observations. Local emission magnitudes and CHBr3:CH2Br2 ratios must be increased more in line with the recent observations of Yokouchi et al. (2005) to improve the model to measurement comparison. Even when the model reproduces the observed bromocarbons, modelled BrO is much less than recent tropical observations (Read et al., 2008). A sea salt source seems the likely explanation. When high BrO is reproduced, the model agrees much better with the observed ozone changes, including diurnal variation, during the measurement period but it is suggested that a representation of iodine chemistry in the model is also required.


2017 ◽  
Vol 17 (18) ◽  
pp. 10919-10935 ◽  
Author(s):  
Yu Wang ◽  
Hao Wang ◽  
Hai Guo ◽  
Xiaopu Lyu ◽  
Hairong Cheng ◽  
...  

Abstract. Over the past 10 years (2005–2014), ground-level O3 in Hong Kong has consistently increased in all seasons except winter, despite the yearly reduction of its precursors, i.e. nitrogen oxides (NOx =  NO + NO2), total volatile organic compounds (TVOCs), and carbon monoxide (CO). To explain the contradictory phenomena, an observation-based box model (OBM) coupled with CB05 mechanism was applied in order to understand the influence of both locally produced O3 and regional transport. The simulation of locally produced O3 showed an increasing trend in spring, a decreasing trend in autumn, and no changes in summer and winter. The O3 increase in spring was caused by the net effect of more rapid decrease in NO titration and unchanged TVOC reactivity despite decreased TVOC mixing ratios, while the decreased local O3 formation in autumn was mainly due to the reduction of aromatic VOC mixing ratios and the TVOC reactivity and much slower decrease in NO titration. However, the decreased in situ O3 formation in autumn was overridden by the regional contribution, resulting in elevated O3 observations. Furthermore, the OBM-derived relative incremental reactivity indicated that the O3 formation was VOC-limited in all seasons, and that the long-term O3 formation was more sensitive to VOCs and less to NOx and CO in the past 10 years. In addition, the OBM results found that the contributions of aromatics to O3 formation decreased in all seasons of these years, particularly in autumn, probably due to the effective control of solvent-related sources. In contrast, the contributions of alkenes increased, suggesting a continuing need to reduce traffic emissions. The findings provide updated information on photochemical pollution and its impact in Hong Kong.


Author(s):  
Charles Halvorson

The passage of the Clean Air Act and the creation of the Environmental Protection Agency (EPA) in 1970 marked a sweeping transformation in American politics. In a few short years, the environmental movement pushed Republican and Democratic elected officials to articulate a right to clean air as part of a bevy of new federal guarantees. Charged with delivering on those promises, the EPA represented a bold assertion that the federal government had a responsibility to protect the environment, the authority to command private business to reduce their pollution, and the capacity to dictate how they did so. But revolutions are always contested and the starburst of environmental concern that propelled the Clean Air Act and the EPA coincided with economic convulsions that shook the liberal state to its core. As powerful businesses pressed to roll back regulations, elected officials from both parties questioned whether the nation could keep its environmental promises. Pushing on, the EPA adopted a monetized approach to environmental value that sat at odds with environmentalist notions of natural rights but provided a critical shield for the agency’s rulemaking, as environmental protection came to serve as a key battleground in larger debates over markets, government, and public welfare. The EPA’s success and the potential limits of its monetary approach are evident in the very air we breathe today—far cleaner and healthier as a result of the EPA’s actions, but holding new threats in a rapidly changing climate.


2016 ◽  
Author(s):  
Mike J. Newland ◽  
Patricia Martinerie ◽  
Emmanuel Witrant ◽  
Detlev Helmig ◽  
David R. Worton ◽  
...  

Abstract. The NOX (NO and NO2) and HOX (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate. However, there remain large uncertainties in the changes to these budgets over recent decades. Due to their short atmospheric lifetimes, NOX and HOX are highly variable in space and time, and so the measurements of these species are of very limited value for examining long term, large scale changes to their budgets. Here, we take an alternative approach by examining long-term atmospheric trends of alkyl nitrates, the formation of which is dependent on the atmospheric NO / HO2 ratio. We derive long term trends in the alkyl nitrates from measurements in firn air from the NEEM site, Greenland. Their mixing ratios increased by a factor of 4–5 between the 1970s and 1990s. This was followed by a steep decline to the sampling date of 2008. Moreover, we examine how the trends in the alkyl nitrates compare to similarly derived trends in their parent alkanes (i.e. the alkanes which, when oxidised in the presence of NOX, lead to the formation of the alkyl nitrates). The ratios of the alkyl nitrates to their parent alkanes increase from around 1970 to the late 1990's consistent with large changes to the [NO] / [HO2] ratio in the northern hemisphere atmosphere during this period. These could represent historic changes to NOX sources and sinks. Alternatively, they could represent changes to concentrations of the hydroxyl radical, OH, or to the transport time of the air masses from source regions to the Arctic.


Sensors ◽  
2018 ◽  
Vol 18 (9) ◽  
pp. 2893 ◽  
Author(s):  
Willem W. Verstraeten ◽  
Klaas Folkert Boersma ◽  
John Douros ◽  
Jason E. Williams ◽  
Henk Eskes ◽  
...  

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April–September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R2 = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R2 = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.


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