Article

Past and future ozone trends in California's South Coast Air Basin: Reconciliation of ambient measurements with past and projected emission inventories

Division of Atmospheric Sciences, Desert Research Institute, Nevada System of Higher Education, Reno, NV 89512, USA.
Journal of the Air & Waste Management Association (1995) (Impact Factor: 1.34). 03/2013; 63(1):54-69. DOI: 10.1080/10962247.2012.735211
Source: PubMed

ABSTRACT

Unlabelled:
This paper updates the historic trends (1980-2010) in ambient ozone and ozone precursor concentrations in the South Coast Air Basin (SoCAB) and examines the evolution of the ozone-precursor relationship in the Basin. Whereas reductions in NOx (oxide of nitrogen) emissions have decreased nitrate and PM2.5 (particulate matter with an aerodynamic diameter < or = 2.5 microm) concentrations in the Basin during the past decade, ozone levels have increased at the central basin locations since about 2005 following a reversal in the decline of volatile organic compound (VOC)/NOx ratios during the previous two decades. A chemical box model was used to simulate the effects of changes in precursor concentrations on ozone formation using day-of-week-specific initial precursor concentrations that were derived from measurements and'projected to 2020 based on expected emission reductions from 2005 (-10% VOC and -50% NOx). Results show that peak ozone formation rates in 2020 will increase on weekdays by a factor of 3 relative to 2005 and will be comparable to 1995 weekday and 2005 Sunday rates. Ozone production will become precursor limited on Sundays in 2020, but with higher initial rates than 2005. Although a greater NOx reduction scenario in 2020 of -75% will result in even higher initial ozone formation rates, precursor limitation is reached quickly, leading to a further shift westward in the location of peak ozone levels. However ozone levels will likely be lower in downwind areas where transport is more important than local production of ozone. The ambient versus emission inventory reconciliation indicates a factor of 2 underestimation of VOC emissions in 2009 relative to NOx. Other analyses suggest that there is an overall increase in VOC emissions on hot days that is not fully accounted for by emission inventory estimates. Air quality models using emission inventories that underestimate VOC emissions relative to NOx may lead to inaccurate forecasting of the consequence of emission reductions.

Implications:
The rate and efficiency of ozone formation and accumulation in the SoCAB is more rapid than would be indicated by air quality model simulations based on the current inventory. Projected reductions in NOx emissions without concurrent reductions in VOC emissions will likely cause ozone to increase during the next decade within central regions of the SoCAB compared with a flat or slightly declining trend in far downwind locations. Air quality statistics that are commonly used to track progress toward attainment, such as basin-wide ozone design value and standard exceedances mask these varying trends within the Basin.

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    • "observed due to reductions in the emission of ozone precursors (Butler et al., 2011; Fiore et al., 1998; Gego et al., 2007; He et al., 2013b; Marufu et al., 2004; Walsh et al., 2008). Numerical simulations of ozone show a dependence on NO x (NO + NO 2 ) concentrations, but do not always capture the regional nature of photochemical smog events nor the strength of the response to NO x emission controls (Fujita et al., 2013; Gilliland et al., 2008; Godowitch et al., 2008a, b; Hogrefe et al., 2011; Pollack et al., 2013; Wilson et al., 2012; Yegorova et al., 2011; Zhou et al., 2013). Recognizing that long-range transport affects local compliance of federally mandated standards, the EPA enacted the Cross State Air Pollution Rule (CSAPR) http://www.epa.gov/crossstaterule which reduces the emissions of ozone precursors from power plants. "
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    ABSTRACT: Regulatory air quality models, such as the Community Multiscale Air Quality model (CMAQ), are used by federal and state agencies to guide policy decisions that determine how to best achieve adherence with National Ambient Air Quality Standards for surface ozone. We use observations of ozone and its important precursor NO2 to test the representation of the photochemistry and emission of ozone precursors within CMAQ. Observations of tropospheric column NO2 from the Ozone Monitoring Instrument (OMI), retrieved by two independent groups, show that the model overestimates urban NO2 and underestimates rural NO2 under all conditions examined for July and August 2011 in the US Northeast. The overestimate of the urban to rural ratio of tropospheric column NO2 for this baseline run of CMAQ (CB05 mechanism, mobile NOx emissions from the National Emissions Inventory; isoprene emissions from MEGAN v2.04) suggests this model may under estimate the importance of interstate transport of NOx. This CMAQ simulation leads to a considerable overestimate of the 2 month average of 8 h daily maximum surface ozone in the US Northeast, as well as an overestimate of 8 h ozone at AQS sites during days when the state of Maryland experienced NAAQS exceedances. We have implemented three changes within CMAQ motivated by OMI NO2 as well as aircraft observations obtained in July 2011 during the NASA DISCOVER-AQ campaign: (a) the modeled lifetime of organic nitrates within CB05 has been reduced by a factor of 10, (b) emissions of NOx from mobile sources has been reduced by a factor of 2, and (c) isoprene emissions have been reduced by using MEGAN v2.10 rather than v2.04. Compared to the baseline simulation, the CMAQ run using all three of these changes leads to a considerably better simulation of the ratio of urban to rural column NO2, better agreement with the 2 month average of daily 8 h maximum ozone in the US Northeast, fewer number of false positives of an ozone exceedance throughout the domain, as well as an unbiased simulation of surface ozone at ground based AQS sites in Maryland that experienced an ozone exceedance during July and August 2007. These modifications to CMAQ may provide a framework for use in studies focused on achieving future adherence to specific air quality standards for surface ozone by reducing emission of NOx from various anthropogenic sectors.
    Full-text · Article · Feb 2015 · Atmospheric Chemistry and Physics
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    • "The annual average trend for secondary ammonium nitrate shows a clear decrease in its concentration , with an approximate 60 and 70% reduction from 2002 to 2013 in Los Angeles and Rubidoux, respectively. This substantial reduction could be in part attributed to a major reduction in NO x emissions in the LA Basin (Fujita et al., 2013), following the implementation of emissions standards after 2007, which targeted NO x as well as PM emissions from diesel trucks. A detailed discussion on the yearly variation of ambient NO x concentrations is provided in the following sections. "
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    ABSTRACT: Positive Matrix Factorization (PMF) was utilized to quantify sources of ambient PM 2.5 in central Los Angeles (LA) and Rubidoux, using the Speciation Trends Network data, collected between 2002 and 2013. Vehicular emissions (including gasoline and diesel vehicles) were the second major contributor to PM 2.5 , following secondary aerosols, with about 20% contribution to total mass in both sites. Starting in 2007, several major federal, state, and local regulations on vehicular emissions were implemented. To assess the effect of these regulations, daily-resolved vehicular source contributions from 2002 to 2006 were pooled together and compared to the combination of 2008 to 2012 datasets. Compared to the 2002 e2006 dataset, the median values of vehicular emissions in 2008e2012 statistically significantly decreased by 24 and 21% in LA and Rubidoux, respectively. These reductions were noted despite an overall increase or similarity in the median values of the daily flow of vehicles after 2007, at the sites.
    Full-text · Article · Jul 2014 · Environmental Pollution
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    • "Although the maximum 8 h average ozone from the individual sites is often less than the basin-wide average, LLS fits of the long-term trends from the individual sites show similar rates of decrease in ozone (average of 3.3 AE 0.2% yr À1 for the five sites shown in Figure 1). We find that the basin-wide data are well fit by a constant exponential decrease of 2.8% yr À1 with no indication of a change in that rate between 1973 and 2010, in contrast to recent descriptions of ozone trends [e.g., Fujita et al., 2013; Warneke et al., 2012] that have invoked a slower rate of decrease in ozone in Los Angeles after 1999. Inclusion of a constant term in the fitting expression to represent a nonnegligible ozone background does not significantly improve the residuals to the data points in Figure 1. "
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    ABSTRACT: [1] Decreases in ozone (O3) observed in California's South Coast Air Basin (SoCAB) over the past five decades have resulted from decreases in local emissions of its precursors, nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs). Ozone precursors have been characterized in the SoCAB with measurements dating back to 1960. Here we compile an extensive historical data set using measurements in the SoCAB between 1960 and 2010. Faster rates of decrease have occurred in abundances of VOCs (−7.3 ± 0.7% yr−1) than in NOx (−2.6 ± 0.3% yr−1), which have resulted in a decrease in VOC/NOx ratio (−4.8 ± 0.9% yr−1) over time. Trends in the NOx oxidation products peroxyacetyl nitrate (PAN) and nitric acid (HNO3), measured in the SoCAB since 1973, show changes in ozone production chemistry resulting from changes in precursor emissions. Decreases in abundances of PAN (−9.3 ± 1.1% yr−1) and HNO3 (−3.0 ± 0.8% yr−1) reflect trends in VOC and NOx precursors. Enhancement ratios of O3 to (PAN + HNO3) show no detectable trend in ozone production efficiency, while a positive trend in the oxidized fraction of total reactive nitrogen (+2.2 ± 0.5% yr−1) suggests that atmospheric oxidation rates of NOx have increased over time as a result of the emissions changes. Changes in NOx oxidation pathways have increasingly favored production of HNO3, a radical termination product associated with quenching the ozone formation cycle.
    Full-text · Article · Jun 2013
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