A Review of Ozone Studies in the Houston ... - ACS Publications

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A Review of Ozone Studies in the Houston−Galveston−Brazoria Nonattainment Area Md. Tarkik Shahriar,1,2 Akhil Kadiyala,1 Raghava Kommalapati,*,1,2 and Ziaul Huque1,3 1Center for Energy & Environmental Sustainability, Prairie View A&M University, Prairie View, Texas 77446, U.S.A. 2Department of Civil & Environmental Engineering, Prairie View A&M University, Prairie View, Texas 77446, U.S.A. 3Department of Mechanical Engineering, Prairie View A&M University, Prairie View, Texas 77446, U.S.A. *E-mail: [email protected].

The United States Environmental Protection Agency identified the Houston-Galveston-Brazoria (HGB) area as a major nonattainment area for ozone (O3) exceedances. Several studies have been reported in the literature that examined the various factors facilitating the O3 exceedances in the HGB area. However, there was no consolidation of research studies representing the HGB area O3 exceedances. This book chapter provides a summary of the findings from research studies associated with O3 exceedances in the HGB area. Based on the literature review, this book chapter noted how the emission of highly reactive volatile organics and nitrogen oxide from industrial facilities in combination with favorable meteorological conditions (e.g., sea breeze circulation, higher solar radiation, weak winds) significantly contributed to O3 exceedances.

© 2015 American Chemical Society Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


Introduction Ozone (O3) is a secondary air pollutant formed through a series of atmospheric chemical reactions in the troposphere. The tropospheric O3 (also referred to as ground-level O3) is formed when two of the precursors, namely, volatile organic compounds (VOCs) and nitrogen oxide (NOx) go through a series of photochemical reactions (1–5). The O3 formation mechanism in troposphere includes the following set of chemical reactions (6). First, reactive VOCs (RH) interact with hydroxyl (OH) radicals to form organic radicals ( ) (reaction 1). Next, the organic radicals combine with molecular oxygen (O2) to form peroxy radicals ( ) (reaction 2). then reacts with nitric oxide (NO) to form nitrogen dioxide (NO2) (reaction 3). In the presence of solar radiation (hv), NO2 is further broken down to form NO and an oxygen atom (O) (reaction 4). Finally, O2 combines with O to form O3 (reaction 5). The O3 formation is a chain reaction process driven by the resulting OH radical formation. The newly formed O3 obtains energy from ultraviolet hv resulting in the development of O (reaction 6). O then reacts with water vapor (H2O) to form two OH radicals (reaction 7). Moreover, further production of OH radicals is possible in the presence of NO, which can be initiated by the RO radical formation (reaction 3). Availability of sufficient VOCs and NOx results in the formation and accumulation of tropospheric O3 as shown by reactions 1 through 7.

Ozone impacts both human health and vegetation. Several studies confirmed a positive relationship between elevated O3 concentrations and premature mortality (7–13). The intake of ground-level O3 can lead to health problems resulting in cough, chest pain, throat congestion and irritation, reduced lung function, and inflammation of linings of the lungs in addition to worsening the conditions of asthma, bronchitis, and emphysema. Agricultural yields of wheat (14, 15), sugar beet (16), potatoes (17), and oilseed rape (18, 19) were observed to be reduced by the phytotoxic properties of O3. Experimental studies have shown 38 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


that the growth and yield of crops (20–23) can be highly affected by existing O3 levels. Several studies (24–32) noted short-term high O3 concentration exposures to be more potent than long-term low O3 concentration exposures with respect to vegetation. The United States Environmental Protection Agency (USEPA) in accordance with the 1990 Clean Air Act set National Ambient Air Quality Standards (NAAQS) for O3 to ensure the safety of public health. The 1990 1-h O3 NAAQS was set to 125 parts per billion (ppb) in accordance with an earlier legislated February 8, 1979 Rule 44 FR 8202. The inability of the 1990 1-h O3 NAAQS to address public health concerns led to the emergence of a more stringent 8-h O3 NAAQS in 1997. The 1997 8-h O3 NAAQS was set to 84 parts per billion (ppb). To determine the O3 attainment status of a particular region, a design value calculated by averaging the fourth-highest 8-h average O3 concentrations across three consecutive years was proposed under the 8-h O3 NAAQS by USEPA. A revision of the 8-h O3 NAAQS was made on March 23, 2008 by reducing the limit from 84 ppb to 75 ppb. The NAAQS are re-evaluated every five years by the USEPA on the basis of best available science to ensure adequate protection of human health. The next revision for 8-h O3 NAAQS, which is currently under review, is proposed to set the limit between 65 ppb and 70 ppb and anticipated to be published as a final rule in October 2015 (33). The Houston-Galveston-Brazoria (HGB) area has been one of the O3 nonattainment areas in the U.S.A. This book chapter is aimed at reviewing existing O3 air quality studies to assess the scope for improvements in developing air quality modeling tools and providing the public with a consolidated summary of O3 studies specifically in the HGB area.

Houston−Galveston−Brazoria Ozone Nonattainment Study Area Figure 1 illustrates the 8-h O3 nonattainment areas based on 2008 NAAQS. A nonattainment area is defined as an area having air pollutant levels persistently exceeding the designated NAAQS levels. The HGB area, geographically located in southeast Texas, consists of eight counties - Brazoria, Chambers, Fort Bend, Galveston, Harris, Liberty, Montgomery, and Waller (refer Figure 2). The HGB area was designated as a severe O3 nonattainment area under the 1997 8-h O3 NAAQS and categorized as a marginal O3 nonattainment area under the 2008 8-h O3 NAAQS. Some studies examined the O3 formation mechanism in the HGB area using photochemical models that simulate air quality based on a set of mathematical equations characterizing the chemical and physical processes. The Comprehensive Air Quality Model with extensions (CAMx) and the Community Multi-scale Air Quality (CMAQ) model are two such photochemical modeling tools adopted by the researchers and regulatory agencies in examining the HGB area O3 formation. Figure 3 illustrates the boundary domain for the HGB area CAMx photochemical modeling grid as specified by Texas Commission on Environmental Quality (TCEQ). The HGB-Beaumont-Port Arthur (HGBPA) modeling subdomain (represented by light blue-colored boundary in Figure 3) has a range (km) with 39 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


(431,505) easting and (-1153,-1079) northing, and is represented by 74 × 74 cells with each cell sizing 1 km × 1 km, within the East Texas Subdomain (represented by green-colored boundary in Figure 3) of the Regional domain (represented by dark blue-colored boundary in Figure 3).

Figure 1. O3 nonattainment areas in the U.S.A. based on 2008 NAAQS. HGB area is represented in blue in southeast Texas. Reproduced with permission from Ref. (34). Copyright (2015) USEPA. (see color insert)

Figure 2. Eight counties in the HGB area. Reproduced with permission from Ref. (35). Copyright (2014) Texas Commission on Environmental Quality. (see color insert) 40 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


Figure 3. CAMx modeling domain grid with HGBPA modeling subdomain (represented by light blue-colored boundary) within the East Texas Subdomain (represented by green-colored boundary) of the Regional domain (represented by dark blue-colored boundary). Reproduced with permission from Ref. (36). Copyright (2014) Texas Commission on Environmental Quality. (see color insert)

Review of Ozone Air Quality Studies in Houston−Galveston−Brazoria Area Daum et al. (37) evaluated and compared the O3 formation rates in two distinct areas within the HGB area: downtown Houston and the Houston Ship Channel. The O3 formation rates in downtown Houston (3-18 ppb/h) were much lower than the O3 formation rates in the Houston Ship Channel (3-80 ppb/h). The higher O3 formation rates in the Houston Ship Channel area are a result of much higher hydrocarbon reactivity (mainly comprising of low molecular weight alkenes). The flight-monitored O3 observations in downtown Houston on August 29, 2000 changed from 30 ppb in the morning to 65 ppb in the early afternoon, and 80 ppb in the late afternoon. The O3 formation in downtown Houston during 41 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


the mornings is driven by point sources such as the Parrish Power Plant located to the southwest of the city. The influence of point sources decreased as the day progressed in downtown Houston. The flight-monitored O3 observations in the Houston Ship Channel on August 29, 2000 were noted to be consistently higher than the O3 observations in downtown Houston by approximately 80 ppb throughout the day and reached a maximum of 180 ppb in the late afternoon. The higher O3 concentrations in the Houston Ship Channel were noted to be a result of a combination of plumes from separate sources. O3 formation in downtown Houston was noted to be much more hydrocarbon limited than in the Houston Ship Channel. Zhou et al. (38) compared the flight-monitored O3 observations in Houston area between 2000 and 2006 summer (August–October) episodes. The averaged O3 concentrations in 2000 and 2006 were noted to be 76 ppb and 58 ppb, respectively. The decrease in O3 concentrations between 2000 and 2006 may be attributed to the implementation of major emission reduction measures undertaken by petrochemical and other sources. The reduction in NOx and highly reactive VOCs (HRVOCs) largely contributed a 40-50% reduction in O3 formation rates from 2000 to 2006. The reduction in HRVOCs also decreased the radical production by 20-50%, further inhibiting the O3 formation rates in Houston. Murphy and Allen (39) extensively studied the hydrocarbon emissions from industrial release events and their associated impact on O3 formation in the Houston-Galveston (HG) area. The “events” or “upsets” were defined as non-routine emissions where the released quantities of those emissions are greater than normal and where such phenomena are observed for a shorter period of time (typically less than 24 h). The online event reporting system, maintained by TCEQ, was used to examine the magnitudes and variability of emission events between January 31, 2003 and January 30, 2004. Flow rates (lb/h) of NOX, VOCs, and HRVOCs were calculated to facilitate computing the magnitude and frequency of those emission events, which were then compared against annual average flow rates within the region and at specific facilities. They identified O3 formation in the HG area to be significantly influenced by the HRVOC emissions and NOX emissions having negligible influence. More than half of the mass of HRVOC event emissions were characterized as ethene, one-third as propene, and the remaining 10% as isomers of butene and 1,3-butadiene. Ethene also dominated the frequency events. There were 761 HRVOC events during the study period, among which 87 (11%) lasted 10 min or less, 192 (25%) lasted 1 h or less, and 567 (75%) lasted 24 h or less. Although the duration of the events was short, their magnitudes were significantly large. In the case of HRVOC events lasting 1 h or less, 33 of the events were reported to release more than 1000 lbs of HRVOCs. Industrial Organic Chemicals were identified to be the primary components accounting for two-thirds of the mass of HRVOC emission events and 90% of the mass in a 12-mo reporting period was attributed to about 20 facilities. Li et al. (40) comprehensively analyzed the impacts of biogenic emissions on photochemical O3 production in the Houston area by applying a three-dimensional regional chemical transport model (CTM) using the Texas Air Quality Study 2000 (TexAQS 2000) database. The simulated O3 concentrations were compared with 42 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


observations from the G-1 research aircraft and a surface-monitoring network. The CTM model performed well in reproducing the location, magnitude, and movements of O3 plumes along with the temporal and geographical variations of O3. The simulated concentrations of total reactive nitrogen (NOy) and the variations of peroxyacetyl nitrate (PAN) from the CTM were in agreement with the monitored observations. Despite the uncertainties that existed in the case of isoprene (an important biogenic hydrocarbon) emissions and meteorological inputs, the CTM simulations compared reasonably with available observations. O3 plume was observed to occur in the urban Houston area in the afternoon, with isoprene emissions playing a major role accounting for approximately 20–40 ppb of O3 concentrations in the Houston area. The study also analyzed the O3 formation by examining the VOC/NO2 reactivity ratios. The VOC/NO2 reactivity ratios were relatively higher in the Houston Ship Channel than in the urban Houston area. This pattern was observed to be opposite for the case of isoprene emissions. When the isoprene emissions were decreased or increased by 50%, the O3 concentrations changed proportionately by 5–25 ppb over the urban Houston area, while the change in the O3 concentration was less than 5–10 ppb over the Houston Ship Channel. Ryerson et al. (41) analyzed the O3 formation potential of petrochemical industrial emissions of reactive alkenes and NOx in the Houston area using two days of TexAQS 2000 database. A three-step approach was adopted. First, the plumes of some geographically isolated complexes (at Freeport, Chocolate Bayou, and Sweeny) were analyzed to evaluate their O3 production potential. Next, data from combined plumes downwind of multiple petrochemical complexes in Texas City area and heavily industrialized Houston Ship Channel were included to study their impact on O3 production potential. Finally, a comparison was made between O3 productions from petrochemical industrial plumes against the observed downwind concentrations of fossil-fueled electric utility power plants in urban/rural areas. Petrochemical emissions’ contribution to O3 formation rates and yields are substantially higher than the contributions of fossil-fueled electric utility power plant emissions. All possible VOCs that are emitted from petrochemical sources were identified to be utilized in O3 production in Houston area. Accurate estimation of reactive light alkenes was noted to be essential in the development of exact VOC emission inventories for Houston petrochemical industrial sources. By decreasing the emissions of ethene and propene, a reduction of over 75% of initial VOC reactivity was observed to have been possible, thereby indicating a reduction in alkene emissions is essential to control O3 exceedances in the Houston area. Washenfelder et al. (42) characterized NOx, sulfur dioxide (SO2), ethene, and propene from industrial emission sources in the Houston area by examining the trends of emissions from industrial sources between 2000 and 2006. HRVOCs were additionally identified using relative OH radical reactivity. The use of abatement controls at industrial facilities provided a reduction of 29% ± 20% (mean ± standard deviation) in NOx emissions between 2000 and 2006. A reduction of 30% ± 30% in emissions of alkenes (ethene, propene) was also observed during the same period. These statistics were based on the examination of temporal trends in ethene/NOx and propene/NOx ratios from 43 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


isolated petrochemical sources. Within the Houston urban area between 2000 and 2006, the median ambient concentrations of ethene and propene have been reduced by 52% and 48%, respectively. The study also identified the continuation of inaccuracies in emission inventory for the 2000, 2002, and 2006 measurements in the HGB area. The emission inventory values exceeded the measured ratios of ethene/NOx and propene/NOx by factors of 1.4–20 and 1–24, respectively. Inaccurate accounting of ethene, propene, and other reactive VOC emissions may have resulted in the difficulty for CTMs to accurately predict O3 levels in the greater Houston area. The study noted the Houston Ship Channel to be the largest source among the many other petrochemical industrial areas (Texas City, Chocolate Bayou, Sweeny, and Freeport) examined. Webster et al. (43) examined the influence of variability in continuous hydrocarbon emissions on O3 formation in the HG area. The methodology involved (a) obtaining a set of observations from various flares and cooling towers and (b) developing models to simulate emission variability using the process of stochastic emissions inventory generation. The impact of industrial point source variability on O3 formation was assessed using CAMx for two episode days in August 2000. A total of 50 sets of stochastic emission inventories were randomly generated with the models for each day resulting in a total of 100 simulations. The maximum increase and decrease in peak O3 concentration was noted to be approximately 10.7 ppb and 4.5 ppb, respectively. These results indicate that the variability in continuous industrial emissions has a significant impact on O3 formation in the HG area. The variability in continuous industrial emissions addresses the variation of O3 concentrations in the HG area by approximately 10–52 ppb. Neuman et al. (44) examined the dependence of photochemical O3 production on oxidation of one of its precursors, NOx, in Houston by evaluating the plumes from the same source region under a variety of meteorological conditions. The study proposed the use of O3 production efficiency (OPE) to calculate the number of O3 molecules formed for each NOx molecule oxidized in analyzing the relationship between photochemical O3 production and NOx oxidation. OPE was calculated by accounting for the influence of changing backgrounds on the measured mixing ratios. Fast response (typically 1 Hz) measurements of PANs, NO2, NO, O3, NOy, carbon monoxide (CO) and nitric acid (HNO3) were analyzed. In plumes downwind from Houston industrial and urban areas, the observed enhancement ratios of ΔO3 and Δ(NOy-NOx) were used to determine OPE. Transport and mixing of pollutants was found to be quite complicated on six daytime flights in Houston. At different times and locations, the plumes were observed to be mixed with the background air pollutants, eventually resulting in varying background concentrations. With an increase in downwind distance, the ratios of ΔCO/ΔNOy and ΔO3/Δ(NOy-NOx) increased. Ratio of ΔO3/Δ(NOy-NOx) was also found to be highly variable and elevated with the change of background concentrations and increment of ΔCO/ΔNOy downwind. Rapid formation of O3 and PANs as well as higher OPE were observed in plumes dominated by Houston Ship Channel emissions. The ratio of O3 to NOx oxidation products ranged between 11 and 12 in the plumes heavily influenced by the Houston Ship Channel as also observed in other studies (41, 45). 44 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


Sarker et al. (46) analyzed the influence of point source VOCs on the HGB air quality by examining the O3 sensitivity with the ratio of hydrogen peroxides (H2O2) to nitric acid (HNO3). The H2O2/HNO3 ratios showed that O3 formation in the HGB area was NOx-limited for the simulated episode, thereby indicating the control of NOx emissions is imperative to control O3 exceedances in the HGB area. VOCs such as acetaldehyde (CH3CHO), formaldehyde (CH2O), ethane (C2H6) and PAN showed good correlation (R2) of 0.81, 0.53, 0.5, and 0.67, respectively with high O3 concentrations. Sulfur dioxide (SO2) had good correlation with VOCs, such as CH3CHO and C2H6 indicating that the reactivity of specific VOC species is significant for O3 exceedances in the HGB area. Xiao et al. (47) noted the HGB O3 formation to be highly nonlinear and dependent on the precursors (NOx, VOC) originating from different emission source categories. Petrochemical facilities in the Houston Ship Channel area were identified as the major sources for both NOx and HRVOC emissions that facilitate rapid and effective O3 formation. The characterized VOC emissions density for different species (CH3CHO, ethene, CH2O, isoprene, olefin carbon bond, paraffin carbon bond, toluene, and xylene) from the Houston Ship Channel and the rest of HGB were noted to be (11.9, 20, 12.5, 0.2, 18.1, 220.9, 18.4, 11.6) and (0.8, 0.8, 0.4, 0.05, 0.9, 13.1, 2.5, 1.9) tons/d/1000 km2, respectively. The CMAQ model sensitivity analysis revealed the Houston Ship Channel petrochemical facilities to be the larger contributors to peak O3 concentrations in the Houston region. NOx emission releases from the Houston Ship Channel (100 tons/d) and other local region sources were also noted to significantly influence the daily peak O3 concentrations. Byun et al. (48) examined the performance of CAMx and CMAQ photochemical models in the case of a high O3 event in the HGB area using same emissions and meteorological data as inputs. The two model simulation results were compared against the aircraft measurements from the TexAQS 2000 study. CMAQ was more assisted by the imputed HRVOC emissions in simulating observed peak O3 concentrations in comparison to CAMx. In some of the highly HRVOC-rich areas, such as downwind of the Houston Ship Channel and other surrounding areas, the O3 peaks predicted by CAMx were found to be higher than those predicted by CMAQ with imputed HRVOC emissions. The study noted the performance of CMAQ system to be essentially poor based on the results of base and imputed case simulations. Sarker et al. (49) analyzed the performance of different chemical mechanisms (CB5, CB6) using CAMx in predicting O3 concentrations in the HGB area. The CAMx CB5 and CB6 results were compared with the observations from TCEQ monitoring stations in the HGB. CB6 chemical mechanism provided better prediction of O3 concentrations than CB5. CB5 O3 predictions were approximately 15% lower than CB6 predictions. Though CB6 improved air quality prediction capacity for CAMx, further modifications are required to accurately predict O3 concentrations. Several studies strived to analyze in detail the influence of meteorology and geographical locations on the HGB area O3 exceedances (42, 50–54). The high levels of O3 in the HGB area are accredited to anthropogenic NOx and VOC sources, which, during the day time of intense solar radiation and stagnant 45 Evans et al.; Trace Materials in Air, Soil, and Water ACS Symposium Series; American Chemical Society: Washington, DC, 2015.


meteorological conditions, combine to form O3 (42). Banta et al. (50) noted that the meteorology of the HGB is favorable for O3 production on the basis of sea breeze circulation that confines the pollutants to the urban area, resulting in accumulation of high levels of O3. Nielson-Gammon et al. (51) noted the months of August and September to be the most susceptible times of the year for high O3 exceedances due to favorable meteorological conditions. Abundant sunshine, high temperatures, weak local winds, and higher frequency of winds from the north during September play a major role in increasing the background O3 in Houston in this time of the year (52). Being located close to the Gulf of Mexico, the HGB is one of the largest Metropolitan areas in the United States that often experiences intense solar radiation during hot and humid summer periods resulting in higher O3 formation (53). The HGB area is by the side of a port with extensive petrochemical production and refining facilities that emit HRVOCs, resulting in higher O3 formation and accumulation compared with other urban areas having a typical mix of anthropogenic emissions (41, 54). The rate of O3 formation in the HGB area can be as high as 200 ppb per hour in contrast to 40 ppb per hour that is the maximum in other urban areas (55).

Conclusions A review of the O3 air quality studies in HGB area was provided. Accurate determination of the sources of the primary O3 precursors, i.e., NOx and VOCs were found to be essential in accurately predicting the O3 exceedances. One of the principle contributors to high O3 exceedances in the HGB area is the emission of HRVOCs and NOx by petrochemical industrial activities around the Houston Ship Channel. The higher industrial emission of VOCs and NOx coupled with favorable meteorology facilitates the rapid formation and accumulation of O3 concentrations. The use of CAMx is recommended for photochemical modeling of O3 concentrations due to its better performance than CMAQ. The use of CAMx with CB6 chemical mechanism proved better prediction and is recommended for use rather than the use of CAMx with CB5 chemical mechanism.

Acknowledgments This work is supported by the National Science Foundation (NSF) through the Center for Energy and Environmental sustainability (CEES), A CREST grant ( #1036593).

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