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Title: U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI)

Abstract

Emissions of nitrogen oxides (NOx) and, subsequently, atmospheric levels of nitrogen dioxide (NO₂) have decreased over the U.S. due to a combination of environmental policies and technological change. Consequently, NO₂ levels have decreased by 30–40% in the last decade. We quantify NO₂ trends (2005–2013) over the U.S. using surface measurements from the U.S. Environmental Protection Agency (EPA) Air Quality System (AQS) and an improved tropospheric NO₂ vertical column density (VCD) data product from the Ozone Monitoring Instrument (OMI) on the Aura satellite.We demonstrate that the current OMI NO₂ algorithm is of sufficient maturity to allow a favorable correspondence of trends and variations in OMI and AQS data. Our trend model accounts for the non-linear dependence of NO₂ concentration on emissions associated with the seasonal variation of the chemical lifetime, including the change in the amplitude of the seasonal cycle associated with the significant change in NOx emissions that occurred over the last decade. The direct relationship between observations and emissions becomes more robust when one accounts for these non-linear dependencies. We improve the OMI NO₂ standard retrieval algorithm and, subsequently, the data product by using monthly vertical concentration profiles, a required algorithm input, from a high-resolution chemistry and transport modelmore » (CTM) simulation with varying emissions (2005-2013). The impact of neglecting the time-dependence of the profiles leads to errors in trend estimation, particularly in regions where emissions have changed substantially. For example, trends calculated from retrievals based on time-dependent profiles offer 18% more instances of significant trends and up to 15% larger total NO₂ reduction versus the results based on profiles for 2005. Using a CTM, we explore the theoretical relation of the trends estimated from NO₂ VCDs to those estimated from ground-level concentrations. The model-simulated trends in VCDs strongly correlate with those estimated from surface concentrations (r = 0.83, N = 355). We then explore the observed correspondence of trends estimated from OMI and AQS data. We find a significant, but slightly weaker, correspondence (i.e., r = 0.68, N = 208) than predicted by the model and discuss some of the important factors affecting the relationship, including known problems (e.g., NOz interferents) associated with the AQS data. This significant correspondence gives confidence in trend and surface concentration estimates from OMI VCDs for locations, such as the majority of the U.S. and globe, that are not covered by surface monitoring networks. Using our improved trend model and our enhanced OMI data product, we find that both OMI and AQS data show substantial downward trends from 2005 to 2013, with an average reduction of 38% for each over the U.S. The annual reduction rates inferred from OMI and AQS measurements are larger (–4.8 ± 1.9%/yr, –3.7 ± 1.5%/yr) from 2005 to 2008 than 2010 to 2013 (–1.2 ± 1.2%/yr, –2.1 ± 1.4%/yr). We quantify NO₂ trends for major U.S. cities and power plants; the latter suggest larger negative trend (–4.0 ± 1.5%/yr) between 2005 and 2008 and smaller or insignificant changes (–0.5 ± 1.2%/yr) during 2010-2013.« less

Authors:
 [1];  [2];  [3];  [2];  [2];  [4];  [4]
+ Show Author Affiliations
  1. Universities Space Research Association, Columbia, MD (United States); NASA Goddard Space Flight Center, Greenbelt, MD (United States)
  2. NASA Goddard Space Flight Center, Greenbelt, MD (United States)
  3. Science Systems and Applications, Inc., Lanham, MD (United States); NASA Goddard Space Flight Center, Greenbelt, MD (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE; National Aeronautics and Space Administration (NASA)
OSTI Identifier:
1196339
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Environment (1994)
Additional Journal Information:
Journal Name: Atmospheric Environment (1994); Journal Volume: 110; Journal Issue: C; Conference: Melbourne (Australia), 19-25 Apr 2015; Journal ID: ISSN 1352-2310
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Lamsal, Lok N., Duncan, Bryan N., Yoshida, Yasuko, Krotkov, Nickolay A., Pickering, Kenneth E., Streets, David G., and Lu, Zifeng. U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI). United States: N. p., 2015. Web. doi:10.1016/j.atmosenv.2015.03.055.
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Lamsal, Lok N., Duncan, Bryan N., Yoshida, Yasuko, Krotkov, Nickolay A., Pickering, Kenneth E., Streets, David G., & Lu, Zifeng. U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI). United States. https://doi.org/10.1016/j.atmosenv.2015.03.055
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Lamsal, Lok N., Duncan, Bryan N., Yoshida, Yasuko, Krotkov, Nickolay A., Pickering, Kenneth E., Streets, David G., and Lu, Zifeng. Mon . "U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI)". United States. https://doi.org/10.1016/j.atmosenv.2015.03.055. https://www.osti.gov/servlets/purl/1196339.
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@article{osti_1196339,
title = {U.S. NO₂ trends (2005–2013): EPA air quality system (AQS) data versus improved observations from the Ozone Monitoring Instrument (OMI)},
author = {Lamsal, Lok N. and Duncan, Bryan N. and Yoshida, Yasuko and Krotkov, Nickolay A. and Pickering, Kenneth E. and Streets, David G. and Lu, Zifeng},
abstractNote = {Emissions of nitrogen oxides (NOx) and, subsequently, atmospheric levels of nitrogen dioxide (NO₂) have decreased over the U.S. due to a combination of environmental policies and technological change. Consequently, NO₂ levels have decreased by 30–40% in the last decade. We quantify NO₂ trends (2005–2013) over the U.S. using surface measurements from the U.S. Environmental Protection Agency (EPA) Air Quality System (AQS) and an improved tropospheric NO₂ vertical column density (VCD) data product from the Ozone Monitoring Instrument (OMI) on the Aura satellite.We demonstrate that the current OMI NO₂ algorithm is of sufficient maturity to allow a favorable correspondence of trends and variations in OMI and AQS data. Our trend model accounts for the non-linear dependence of NO₂ concentration on emissions associated with the seasonal variation of the chemical lifetime, including the change in the amplitude of the seasonal cycle associated with the significant change in NOx emissions that occurred over the last decade. The direct relationship between observations and emissions becomes more robust when one accounts for these non-linear dependencies. We improve the OMI NO₂ standard retrieval algorithm and, subsequently, the data product by using monthly vertical concentration profiles, a required algorithm input, from a high-resolution chemistry and transport model (CTM) simulation with varying emissions (2005-2013). The impact of neglecting the time-dependence of the profiles leads to errors in trend estimation, particularly in regions where emissions have changed substantially. For example, trends calculated from retrievals based on time-dependent profiles offer 18% more instances of significant trends and up to 15% larger total NO₂ reduction versus the results based on profiles for 2005. Using a CTM, we explore the theoretical relation of the trends estimated from NO₂ VCDs to those estimated from ground-level concentrations. The model-simulated trends in VCDs strongly correlate with those estimated from surface concentrations (r = 0.83, N = 355). We then explore the observed correspondence of trends estimated from OMI and AQS data. We find a significant, but slightly weaker, correspondence (i.e., r = 0.68, N = 208) than predicted by the model and discuss some of the important factors affecting the relationship, including known problems (e.g., NOz interferents) associated with the AQS data. This significant correspondence gives confidence in trend and surface concentration estimates from OMI VCDs for locations, such as the majority of the U.S. and globe, that are not covered by surface monitoring networks. Using our improved trend model and our enhanced OMI data product, we find that both OMI and AQS data show substantial downward trends from 2005 to 2013, with an average reduction of 38% for each over the U.S. The annual reduction rates inferred from OMI and AQS measurements are larger (–4.8 ± 1.9%/yr, –3.7 ± 1.5%/yr) from 2005 to 2008 than 2010 to 2013 (–1.2 ± 1.2%/yr, –2.1 ± 1.4%/yr). We quantify NO₂ trends for major U.S. cities and power plants; the latter suggest larger negative trend (–4.0 ± 1.5%/yr) between 2005 and 2008 and smaller or insignificant changes (–0.5 ± 1.2%/yr) during 2010-2013.},
doi = {10.1016/j.atmosenv.2015.03.055},
journal = {Atmospheric Environment (1994)},
number = C,
volume = 110,
place = {United States},
year = {Mon Jun 01 00:00:00 EDT 2015},
month = {Mon Jun 01 00:00:00 EDT 2015}
}
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    journal, January 2016

    • Laughner, Joshua L.; Zare, Azimeh; Cohen, Ronald C.
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 23
    • DOI: 10.5194/acp-16-15247-2016

    A high-resolution and observationally constrained OMI NO 2 satellite retrieval
    journal, January 2017

    • Goldberg, Daniel L.; Lamsal, Lok N.; Loughner, Christopher P.
    • Atmospheric Chemistry and Physics, Vol. 17, Issue 18
    • DOI: 10.5194/acp-17-11403-2017

    A physics-based approach to oversample multi-satellite, multispecies observations to a common grid
    journal, January 2018

    • Sun, Kang; Zhu, Lei; Cady-Pereira, Karen
    • Atmospheric Measurement Techniques, Vol. 11, Issue 12
    • DOI: 10.5194/amt-11-6679-2018

    Assessment of NO2 observations during DISCOVER-AQ and KORUS-AQ field campaigns
    journal, January 2020

    • Choi, Sungyeon; Lamsal, Lok N.; Follette-Cook, Melanie
    • Atmospheric Measurement Techniques, Vol. 13, Issue 5
    • DOI: 10.5194/amt-13-2523-2020

    Nitrogen Oxides Emissions, Chemistry, Deposition, and Export Over the Northeast United States During the WINTER Aircraft Campaign
    journal, November 2018

    • Jaeglé, L.; Shah, V.; Thornton, J. A.
    • Journal of Geophysical Research: Atmospheres, Vol. 123, Issue 21
    • DOI: 10.1029/2018jd029133

    Decadal changes in summertime reactive oxidized nitrogen and surface ozone over the Southeast United States
    journal, January 2018

    • Li, Jingyi; Mao, Jingqiu; Fiore, Arlene M.
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 3
    • DOI: 10.5194/acp-18-2341-2018

    Using satellite observations of tropospheric NO 2 columns to infer long-term trends in US NO x emissions: the importance of accounting for the free tropospheric NO 2 background
    journal, January 2019

    • Silvern, Rachel F.; Jacob, Daniel J.; Mickley, Loretta J.
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 13
    • DOI: 10.5194/acp-19-8863-2019

    Fine-Scale Columnar and Surface NOx Concentrations over South Korea: Comparison of Surface Monitors, TROPOMI, CMAQ and CAPSS Inventory
    journal, January 2020

    Quantification of the effect of modeled lightning NO 2 on UV–visible air mass factors
    journal, January 2017

    • Laughner, Joshua L.; Cohen, Ronald C.
    • Atmospheric Measurement Techniques, Vol. 10, Issue 11
    • DOI: 10.5194/amt-10-4403-2017

    Satellite NO2 retrievals suggest China has exceeded its NOx reduction goals from the twelfth Five-Year Plan
    journal, October 2016

    • de Foy, Benjamin; Lu, Zifeng; Streets, David G.
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep35912

    Unexpected slowdown of US pollutant emission reduction in the past decade
    journal, April 2018

    • Jiang, Zhe; McDonald, Brian C.; Worden, Helen
    • Proceedings of the National Academy of Sciences, Vol. 115, Issue 20
    • DOI: 10.1073/pnas.1801191115

    The Ozone Monitoring Instrument: overview of 14 years in space
    journal, January 2018

    • Levelt, Pieternel F.; Joiner, Joanna; Tamminen, Johanna
    • Atmospheric Chemistry and Physics, Vol. 18, Issue 8
    • DOI: 10.5194/acp-18-5699-2018

    The benefits of lower ozone due to air pollution emission reductions (2002–2011) in the Eastern United States during extreme heat
    journal, January 2020

    • Loughner, Christopher P.; Follette-Cook, Melanie B.; Duncan, Bryan N.
    • Journal of the Air & Waste Management Association, Vol. 70, Issue 2
    • DOI: 10.1080/10962247.2019.1694089

    Characterization of ozone production in San Antonio, Texas, using measurements of total peroxy radicals
    journal, January 2019

    • Anderson, Daniel C.; Pavelec, Jessica; Daube, Conner
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 5
    • DOI: 10.5194/acp-19-2845-2019

    Comparison of TROPOMI/Sentinel-5 Precursor NO2 observations with ground-based measurements in Helsinki
    journal, January 2020

    • Ialongo, Iolanda; Virta, Henrik; Eskes, Henk
    • Atmospheric Measurement Techniques, Vol. 13, Issue 1
    • DOI: 10.5194/amt-13-205-2020

    Evaluating a Space-Based Indicator of Surface Ozone-NO x -VOC Sensitivity Over Midlatitude Source Regions and Application to Decadal Trends : Space-Based Indicator of O
    journal, October 2017

    • Jin, Xiaomeng; Fiore, Arlene M.; Murray, Lee T.
    • Journal of Geophysical Research: Atmospheres, Vol. 122, Issue 19
    • DOI: 10.1002/2017jd026720

    Aura OMI observations of regional SO 2 and NO 2 pollution changes from 2005 to 2015
    journal, January 2016

    • Krotkov, Nickolay A.; McLinden, Chris A.; Li, Can
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 7
    • DOI: 10.5194/acp-16-4605-2016

    NH3 emissions from large point sources derived from CrIS and IASI satellite observations
    journal, January 2019

    • Dammers, Enrico; McLinden, Chris A.; Griffin, Debora
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 19
    • DOI: 10.5194/acp-19-12261-2019

    Comparing OMI-based and EPA AQS in situ NO2 trends: towards understanding surface NOx emission changes
    journal, January 2018

    • Zhang, Ruixiong; Wang, Yuhang; Smeltzer, Charles
    • Atmospheric Measurement Techniques, Vol. 11, Issue 7
    • DOI: 10.5194/amt-11-3955-2018

    A space-based, high-resolution view of notable changes in urban NO x pollution around the world (2005-2014) : NOTABLE CHANGES IN URBAN NO
    journal, January 2016

    • Duncan, Bryan N.; Lamsal, Lok N.; Thompson, Anne M.
    • Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 2
    • DOI: 10.1002/2015jd024121

    A top-down assessment using OMI NO 2 suggests an underestimate in the NO x emissions inventory in Seoul, South Korea, during KORUS-AQ
    journal, January 2019

    • Goldberg, Daniel L.; Saide, Pablo E.; Lamsal, Lok N.
    • Atmospheric Chemistry and Physics, Vol. 19, Issue 3
    • DOI: 10.5194/acp-19-1801-2019

    Microbial mechanisms and ecosystem flux estimation for aerobic NO y emissions from deciduous forest soils
    journal, January 2019

    • Mushinski, Ryan M.; Phillips, Richard P.; Payne, Zachary C.
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 6
    • DOI: 10.1073/pnas.1814632116

    Emissions of nitrogen oxides from US urban areas: estimation from Ozone Monitoring Instrument retrievals for 2005–2014
    journal, January 2015

    Improved slant column density retrieval of nitrogen dioxide and formaldehyde for OMI and GOME-2A from QA4ECV: intercomparison, uncertainty characterisation, and trends
    journal, January 2018

    • Zara, Marina; Boersma, K. Folkert; De Smedt, Isabelle
    • Atmospheric Measurement Techniques, Vol. 11, Issue 7
    • DOI: 10.5194/amt-11-4033-2018

    The benefits of lower ozone due to air pollution emission reductions (2002–2011) in the Eastern US during extreme heat
    text, January 2020

    Emissions of nitrogen oxides from US urban areas: estimation from Ozone Monitoring Instrument retrievals for 2005–2014
    journal, January 2015

    • Lu, Z.; Streets, D. G.; de Foy, B.
    • Atmospheric Chemistry and Physics Discussions, Vol. 15, Issue 10
    • DOI: 10.5194/acpd-15-14961-2015
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