Ozone production efficiency and loss of NOx in power plant plumes: Photochemical model and interpretation of measurements in Tennessee

Sillman, Sanford

doi:10.1029/1999jd901014

Cited by 61 publications

(67 citation statements)

References 39 publications

(32 reference statements)

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“…The OPE values relative to NO z calculated from the BORTAS measurements represent the extremes of typical OPE values previously reported in the literature and summarised in Table 1 of Rickard et al (2002). The OPE of 1.6 ppbv ppbv −1 relative to NO z in the BOR-TAS plume measurements with high aerosol loading is similar to the OPE observed in urban and power station pollution plumes in the eastern USA (Chin et al, 1994;Ryerson et al, 1998;Daum et al, 2000;Sillman, 2000) whereas the OPE of 155 ppbv ppbv −1 in the plume measurements with low aerosol loading is more comparable to the OPE observed in aged air masses of continental origin over the western Pacific Ocean (Davis et al, 1996).…”

Section: Ozone Production Efficiencymentioning

confidence: 54%

Ozone photochemistry in boreal biomass burning plumes

et al. 2013

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We present an analysis of ozone (O₃) photochemistry observed by aircraft measurements of boreal biomass burning plumes over eastern Canada in the summer of 2011. Measurements of O₃ and a number of key chemical species associated with O₃ photochemistry, including non-methane hydrocarbons (NMHCs), nitrogen oxides (NO_x) and total nitrogen containing species (NO_y), were made from the UK FAAM BAe-146 research aircraft as part of the "quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS) experiment between 12 July and 3 August 2011. The location and timing of the aircraft measurements put BORTAS into a unique position to sample biomass burning plumes from the same source region in Northwestern Ontario with a range of ages. We found that O₃ mixing ratios measured in biomass burning plumes were indistinguishable from non-plume measurements, but evaluating them in relationship to measurements of carbon monoxide (CO), total alkyl nitrates (ΣAN) and the surrogate species NO_z (= NO_y-NO_x) revealed that the potential for O₃ production increased with plume age. We used NMHC ratios to estimate photochemical ages of the observed biomass burning plumes between 0 and 10 days. The BORTAS measurements provided a wide dynamic range of O₃ production in the sampled biomass burning plumes with ΔO₃/ΔCO enhancement ratios increasing from 0.020 ± 0.008 ppbv ppbv⁻¹ in plumes with photochemical ages less than 2 days to 0.55 ± 0.29 ppbv ppbv⁻¹ in plumes with photochemical ages greater than 5 days. We found that the main contributing factor to the variability in the ΔO₃/ΔCO enhancement ratio was ΔCO in plumes with photochemical ages less than 4 days, and that was a transition to ΔO₃ becoming the main contributing factor in plumes with ages greater than 4 days. In comparing O₃ mixing ratios with components of the NO_y budget, we observed that plumes with ages between 2 and 4 days were characterised by high aerosol loading, relative humidity greater than 40%, and low ozone production efficiency (OPE) of 7.7 ± 3.5 ppbv ppbv⁻¹ relative to ΣAN and 1.6 ± 0.9 ppbv ppbv⁻¹ relative to NO_z. In plumes with ages greater than 4 days, OPE increased to 472 ± 28 ppbv ppbv⁻¹ relative to ΣAN and 155 ± 5 ppbv ppbv⁻¹ relative to NO_z. From the BORTAS measurements we estimated that aged plumes with low aerosol loading were close to being in photostationary steady state and O₃ production in younger plumes was inhibited by high aerosol loading and greater production of ΣAN relative to O₃. The BORTAS measurements of O₃ photochemistry in boreal biomass burning plumes were found to be consistent with previous summertime aircraft measurements made over the same region during the Arctic Research of the Compos...

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Section: Ozone Production Efficiencymentioning

confidence: 54%

Ozone photochemistry in boreal biomass burning plumes

et al. 2013

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“…From a pollution point of view, all regions are similar to the conditions encountered over the Swiss Plateau. For an assumed temperature of 298 K and based on OH concentrations taken from the BERLIOZ and the SLOPE96 campaigns with noontime values of (4-8)×10 6 cm −3 (Volz- Mihelcic et al, 2003) and (7-10)×10 6 cm −3 (Volz-Thomas and Kolahgar, 2000), respectively, the resulting mean daytime NO x lifetimes in summer are estimated to be 4.6 h and 3.0 h. These data have been deduced from campaigns in the U.S. (Spicer, 1982;Ryerson et al, 1998;Nunnermacker et al, 2000;Sillman, 2000) and in the Swiss Plateau (Dommen et al, 1999), from GOME NO 2 VTCs over Germany (Beirle et al, 2003) and from the GEOS-CHEM model (Fig. 7).…”

Section: No X Lifetime Under Anticyclonic Clear Sky Conditionsmentioning

confidence: 99%

SCIAMACHY tropospheric NO2 over Switzerland: estimates of NOx lifetimes and impact of the complex Alpine topography on the retrieval

et al. 2007

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Abstract. This study evaluates NO 2 vertical tropospheric column densities (VTCs) retrieved from measurements of the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) above Switzerland and the Alpine region. The close correlation between pixel averaged NO x emission rates from a spatially and temporally highly resolved inventory and the NO 2 VTCs under anticyclonic meteorological conditions demonstrates the general ability of SCIAMACHY to detect sources of NO x pollution in Switzerland. This correlation is further used to infer seasonal mean NO x lifetimes carefully taking into account the influence of the strong diurnal cycle in NO x emissions on these estimates. Lifetimes are estimated to 3.6 (±0.8) hours in summer and 13.1 (±3.8) hours in winter, the winter value being somewhat lower than previous estimates. A comparison between the 2003-2005 mean NO 2 VTC distribution over Switzerland and the corresponding 1996-2003 mean from the Global Ozone Monitoring Experiment (GOME) illustrates the much better capability of SCIAMACHY to resolve regional scale pollution features. However, the comparison of seasonal averages over the Swiss Plateau with GOME and ground based in situ observations indicates that SCIAMACHY exhibits a too weak seasonal cycle with comparatively high values in summer and low values in winter. A problem likely contributing to the reduced values in winter (not reported in earlier literature) is the use of inaccurate satellite pixel surface pressures derived from a coarse resolution global model in the retrieval. The marked topography in the Alpine region can lead to deviations of several hundred meters between the model assumed and the real pixel-averaged surface height. A Correspondence to: D. Brunner (dominik.brunner@empa.ch) sensitivity study based on selected clear sky SCIAMACHY NO 2 VTCs over the Swiss Plateau and two fixed a priori NO 2 profile shapes indicates that inaccurate pixel surface pressures affect retrieved NO 2 columns over complex terrain by up to 40%. For retrievals in the UV-visible spectral range with a decreasing sensitivity towards the earth's surface, this effect is of major importance when the NO 2 resides close to the ground, a situation most frequently observed during winter.

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“…From the data of O x (≡O 3 + NO 2 ) and NO z , the ratio of (O z )/ (NO z ) can be calculated and considered to be a kind of observation-based OPE (Olszyna et al, 1994;Sillman, 2000;Trainer et al, 1993;Kleinman et al, 2002;Nunnermacker et al, 1998). Figure 10 shows the time series of daily OPEx during the observation period.…”

Section: Photochemical Aging and Ozone Production Efficiencymentioning

confidence: 99%

Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological, and chemical impacts

Lin

et al. 2011

Atmos. Chem. Phys.

120

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Abstract. Gaseous pollutants, NO y /NO x , SO 2 , CO, and O 3 , were measured at an urban site in Beijing from 17 November 2007 to 15 March 2008. The average concentrations (with ± 1σ ) of NO, NO 2 , NO x , NO y , CO, SO 2 , and O 3 were 29.0 ± 2.7 ppb, 33.7 ± 1.4 ppb, 62.7 ± 4.0 ppb, 72.8 ± 4.5 ppb, 1.99 ± 0.13 ppm, 31.9 ± 2.0 ppb, and 11.9 ± 0.8 ppb, respectively, with hourly maxima of 200.7 ppb, 113.5 ppb, 303.9 ppb, 323.2 ppb, 15.06 ppm, 147.3 ppb, and 69.7 ppb, respectively. The concentrations of the pollutants show "saw-toothed" patterns, which are attributable mainly to changes in wind direction and speed. The frequency distributions of the hourly mean concentrations of NO y , SO 2 , CO, and O 3 can all be decomposed in the two Lorentz curves, with their peak concentrations representing background levels under different conditions. During the observation period, the average ratio NO x /NO y was 0.86 ± 0.10, suggesting that the gaseous pollutants in Beijing in winter are mainly from local emissions. Data of O 3 , NO z , and NO x /NO y indicate that photochemistry can take place in Beijing even in the cold winter period. Based on the measurements of O 3 , NO x , and NO y , ozone production efficiency (OPE) is estimated to be in the range of 0-8.9 (ppb ppb −1 ) with the mean(±1σ ) and median values being 1.1(±1.6) and 0.5 (ppb ppb −1 ), respectively, for the winter 2007-2008 in Beijing. This low OPE would cause a photochemical O 3 source of 5 ppb day −1 , which is small but significant for surface O 3 in winter in Beijing.Correspondence to: X. Xu (xuxb@cams.cma.gov.cn) Downward transport of O 3 -rich air from the free troposphere is the more important factor for the enhancement of the O 3 level in the surface layer, while high NO level for the destruction of O 3 . The concentrations of SO 2 , CO, and NO x are strongly correlated among each other, indicating that they are emitted by some common sources. Multiple linear regression analysis is applied to the concentrations of NO y , SO 2 , and CO and empirical equations are obtained for the NO y concentration. Based the equations, the relative contributions from mobile and point sources to NO y is estimated to be 66 ± 30 % and 40 ± 16 %, respectively, suggesting that even in the heating period, mobile sources in Beijing contribute more to NO y than point sources.

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Ozone production efficiency and loss of NO_x in power plant plumes: Photochemical model and interpretation of measurements in Tennessee

Cited by 61 publications

References 39 publications

Ozone photochemistry in boreal biomass burning plumes

Ozone photochemistry in boreal biomass burning plumes

SCIAMACHY tropospheric NO<sub>2</sub> over Switzerland: estimates of NO<sub>x</sub> lifetimes and impact of the complex Alpine topography on the retrieval

Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological, and chemical impacts

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Ozone production efficiency and loss of NOx in power plant plumes: Photochemical model and interpretation of measurements in Tennessee

Cited by 61 publications

References 39 publications

Ozone photochemistry in boreal biomass burning plumes

Ozone photochemistry in boreal biomass burning plumes

SCIAMACHY tropospheric NO&lt;sub&gt;2&lt;/sub&gt; over Switzerland: estimates of NO&lt;sub&gt;x&lt;/sub&gt; lifetimes and impact of the complex Alpine topography on the retrieval

Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological, and chemical impacts

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Ozone production efficiency and loss of NO_x in power plant plumes: Photochemical model and interpretation of measurements in Tennessee

SCIAMACHY tropospheric NO<sub>2</sub> over Switzerland: estimates of NO<sub>x</sub> lifetimes and impact of the complex Alpine topography on the retrieval