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atmosphere

Article Winter Ozone Pollution in ’s is Attenuating

Marc L. Mansfield * and Seth N. Lyman

Department of Chemistry and Biochemistry, Utah State University Uintah Basin, 320 North Aggie Boulevard, Vernal, UT 84078, USA; [email protected] * Correspondence: marc.mansfi[email protected]

Abstract: High concentrations of ground-level ozone have been observed during wintertime in the Uinta Basin of western Utah, USA, beginning in 2010. We analyze existing ozone and ozone precursor concentration data from 38 sites over 11 winter seasons and conclude that there has been a statistically significant (p < 0.02) decline in ozone concentration over the previous decade. Daily exceedances of the National Ambient Air Quality Standard for ozone (70 ppb) have been trending downward at the rate of nearly four per year. Ozone and NOx concentrations have been trending downward at the rates of about 3 and 0.3 ppb per year, respectively. Concentrations of organics in 2018 were at about 30% of their values in 2012 or 2013. Several markers, annual ozone exceedance counts and median ozone and NOx concentrations, were at their largest values in the period 2010 to 2013 and have never recovered since then. We attribute the decline to (1) weakening global demand for oil and natural gas and (2) more stringent pollution regulations and controls, both of which have occurred over the previous decade. We also see evidence of ozone titration when snow cover is absent.

Keywords: winter ozone; data analysis; Uinta Basin; Utah

1. Introduction Many winters in the Uinta Basin of eastern Utah display high concentrations of   ground-level ozone. The Basin is one of only two regions worldwide in which winter ozone concentrations consistently above background and consistently above the National Citation: Mansfield, M.L.; Lyman, S.N. Ambient Air Quality Standard (NAAQS) for ozone, 70 ppb, have been observed. (The other Winter Ozone Pollution in Utah’s Uinta is the Upper Green River Basin in western , about 300 km to the north.) Winter Basin is Attenuating. Atmosphere 2021, ozone always occurs in conjunction with persistent, multi-day thermal inversions; an active 12, 4. https://dx.doi.org/10.3390/ atmos12010004 oil and natural gas extraction industry; and in the presence of a snowpack. The industry produces ozone precursors, the inversions trap these precursors within the inversion

Received: 17 November 2020 layer, and the snow surface albedo provides sufficient actinic flux for ozone formation Accepted: 17 December 2020 to occur [1–8]. Published: 23 December 2020 Because of the changing solar elevation, high ozone episodes are less frequent near the winter solstice and become more frequent in January and February. The episodes also Publisher’s Note: MDPI stays neu- end with the disappearance of the snowpack, usually during the first or second week of tral with regard to jurisdictional claims March [2–5]. The Uinta Basin lies in a snow shadow cast by the surrounding mountains and in published maps and institutional receives fewer storms than surrounding regions. Nevertheless, snow cover from a single affiliations. significant snowstorm, usually in December, is adequate to stabilize cold pool inversions for the remainder of the season and usually guarantees that the snowpack will not melt until March. But without that one significant snowstorm, we typically see little or no snow throughout the season, and ozone usually remains near background values (see below). Copyright: © 2020 by the authors. Li- The Uinta and Upper Green River Basins are rural, and exhibit only occasional censee MDPI, Basel, Switzerland. This ozone exceedances in summer (often as a result of stratospheric intrusions or wildfires). article is an open access article distributed under the terms and conditions of the On the other hand, there are urban valleys and basins in the western USA with frequent Creative Commons Attribution (CC BY) summer ozone exceedances that do not produce ozone in winter, even though they may license (https://creativecommons.org/ have snowpacks, persistent inversions, and ozone precursor sources [9]. A possible hy- licenses/by/4.0/). pothesis to explain this difference is that the precursor speciation mix from urban sources

Atmosphere 2021, 12, 4. https://dx.doi.org/10.3390/atmos12010004 https://www.mdpi.com/journal/atmosphere Atmosphere 2021, 12, 4 2 of 18

is different than that from the petroleum extraction industry. Temperature and absolute humidity differences probably also contribute. A quantifiable definition of inversion strength is needed to correlate high ozone with thermal inversion episodes. This is problematic for the Uinta Basin, because temperature– altitude profiles are not measured routinely. But the variation in surface temperature with altitude also indicates inversion strength. Therefore, we define a daily “pseudo-lapse rate,” Ψ, from the slope of the least-squares line obtained from plots of daily maximum surface temperature vs. altitude at a number of sites throughout the Basin [9–11]. Because of a number of confounding factors, especially differences in ambient meteo- rology from one season to the next, it has been difficult in the past to observe any long-term trends in the ozone data. However, the present analysis indicates that winter ozone and pre- cursor concentrations in the Uinta Basin have displayed a statistically significant (p < 0.02) attenuation over the past decade. The purpose of this paper is to document these trends in the data. The two most likely causes for this attenuation are (1) the contraction of the Basin’s oil and natural gas industry caused by a generally weakening market demand, and (2) pollution controls on oil and natural gas production that have come online over the past decade.

2. Methods 2.1. Ozone Concentration Data In this paper, unless indicated otherwise, we define ozone season S as extending from 15 December in year S − 1 to March 15 of year S. Over all the years for which data are available, these two dates always bracket exceedances of the NAAQS that can be attributed to the winter ozone phenomenon. Data, in the form of the daily maximum in the eight-hour running average of ozone concentrations, were obtained from two sources: (1) The US Environmental Protection Agency AQS datasite contains data contributed by a number of agencies, including the US Environmental Protection Agency, the US National Park Service, the US Forest Service, the Utah Division of Air Quality, and the Ute Indian Tribe [12]. (2) Our group at Utah State University (USU) has for many years measured and archived ozone concentrations from many sites throughout the Uinta Basin, using Model 205 Dual Beam Ozone Monitors manufactured by 2B Technologies [2–5,8]. Using both sources, we were able to assemble an ozone concentration dataset from 38 different sites over eleven years. Many sites only provide coverage for one or a few seasons, but three cover all seasons from 2011 to 2019, six more from 2011 to 2020, and two more from 2010 to 2020. Metadata about the sites are given in the Supplementary Material.

2.2. Ozone Precursor Measurements We also have routine measurements of ozone precursor concentrations beginning in 2010 at a number of sites, as summarized in the Supplementary Material. NOx measure- ments are available at two sites from 2010 to 2020, four sites from 2012 to 2020, and one more site from 2013 to 2020. As with ozone, NOx data were either obtained from the US EPA AQS datasite [12] or our own measurement archive. Most available NOx measure- ments were made with conventional molybdenum oxide NO2 converters. Molybdenum oxide converters are well known to result in a high NO2 bias when concentrations of other reactive nitrogen compounds (e.g., HNO3, HNO2, organic nitrates, etc.; often abbreviated as NOz) are high [13–15]. Two USU-operated stations use ultraviolet light-based NO2 converters, which are not subject to this bias [14]. Figure1 shows the difference between measurements at one of those stations and co-located measurements collected with a molybdenum oxide converter. High concentrations of NOz that lead to the bias only occur during inversion events with elevated ozone concentrations, so this bias can be expected to be minimal on days when the pseudo-lapse rate is above zero. Atmosphere 2021, 12, x FOR PEER REVIEW 3 of 19

Atmosphere 2021, 12, 4 3 of 18 during inversion events with elevated ozone concentrations, so this bias can be expected to be minimal on days when the pseudo-lapse rate is above zero.

FigureFigure 1. 1. DifferenceDifference between NO 22 measuredmeasured with with an an instrument utilizing a molybdenum oxide NO2 converter and NO 2 measuredmeasured with anan instrumentinstrument utilizing utilizing a a UV UV photolytic photolytic converter converter versus versus NO NOz atz the at Rooseveltthe Roosevelt monitoring monitoring station. station. Theblack The blackline shows line shows a linear a linear regression regression curve cu forrve the for relationship. the relationship. From From [16]. [16].

MeasurementsMeasurements of of organic organic compounds compounds have have been been less less plentiful plentiful and and less less consistent consistent in in thethe Uinta Uinta Basin. Basin. The The only only multi-year multi-year time time series series of of organics organics that that exist exist are are at at the the Horsepool Horsepool andand Roosevelt Roosevelt monitoring monitoring stations. stations. At At Hors Horsepool,epool, organic organic compound compoundss were were measured measured by carbon-trapby carbon-trap concentration/thermal concentration/thermal desorption desorption,, gas chromatograph gas chromatograph (GC) (GC)separation, separation, and massand massspectrometer spectrometer (MS) (MS) or flame or flame ionization ionization detector detector (FID) (FID) by by a ateam team from from the the National National OceanicOceanic and and Atmospheric AdministrationAdministration inin winters winters 2012, 2012, 2013, 2013, and and 2014 2014 [3 ,[3,17–20].17–20]. During Dur- ingwinters winters 2017–2020, 2017–2020, we we collected collected daily daily three-hour three-hour canister canister samples sample (beginnings (beginning at midnight at mid- nightor noon). or noon). We concentrated We concentrated organic organic compounds compounds in the canisters in the canisters using cold using trap cold dehydration, trap de- hydration,and we analyzed and we themanalyzed via GC-GC-FID/MSthem via GC-GC- [FID/MS21]. At Roosevelt,[21]. At Roosevelt, we measured we measured organic organiccompounds compounds with a Perkin with a ElmerPerkin TurboMatrix Elmer TurboMatrix TD thermal TD thermal desorption desorption system and system a Clarus and a580 Clarus GC-FID 580 duringGC-FID winters during 2013winters and 2013 2015 and [19]. 2015 During [19]. winters During 2017–2020, winters 2017–2020, we collected we collecteddaily three-hour daily three-hour canister samplescanister samples and analyzed and analyzed the samples the samples as at Horsepool as at Horsepool [21]. [21].

2.3.2.3. Measurement Measurement Quality Quality Assurance Assurance Measurements obtained from the US EPA AQS database [12] meet quality assurance Measurements obtained from the US EPA AQS database [12] meet quality assurance criteria determined by EPA and the organizations that collected the data. Data collected by criteria determined by EPA and the organizations that collected the data. Data collected USU were only included in this analysis if they met quality assurance criteria outlined in by USU were only included in this analysis if they met quality assurance criteria outlined our management plan [22] and included the following criteria: For ozone, NOx, and NOy, in our management plan [22] and included the following criteria: For ozone, NOx, and we performed three-point calibration checks at least every two weeks, requiring ±5% NOy, we performed three-point calibration checks at least every two weeks, requiring ±5% accuracy. For organic compound canisters we performed pressure testing for leaks on each accuracy. For organic compound canisters we performed pressure testing for leaks on canister between field retrieval and the gas chromatograph runs. Quality assurance results each canister between field retrieval and the gas chromatograph runs. Quality assurance for each measurement year are available in USU’s annual Uinta Basin air quality research reports [2–4,8,16,19–21,23,24].

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2.4. Pseudo-Lapse Rate and Snowdepth We downloaded daily maximum surface temperatures at sites throughout the Uinta Basin from the Utah Climate Center website [25]. The Center accesses the Global Historical Climatology Network (GHCN), the Global Summary of the Day (GSOD) data, the National Weather Service’s Cooperative Observer Program (COOP), and other sources. We in- cluded all available data from stations within the Basin over the time period of interest (2009 to 2020) at altitudes lower than 2000 m. (Stations at higher than 2000 m tend to lie in the non-linear part of the temperature–altitude profile and bias the calculation [11].) The daily pseudo-lapse rate, Ψ, is the negative slope of the least-squares line used to fit the temperature–altitude data: Ψ = −∂T/∂z. We have also applied this definition in other studies [9–11]. Many of the databases also report a daily snowdepth. We calculated the basin-average snowdepth by averaging over all stations at altitudes below 2000 m that reported a snowdepth.

2.5. Data on Oil and Natural Gas Production We accessed a database maintained by the Utah Division of Oil, Gas, and Mining for the coordinates and production statistics of all active oil and natural gas wells in the Basin, and statistics on the drilling of new wells [26].

3. Results 3.1. Correlations between Snow Cover and Ozone Formation Figure2 displays the average ozone concentration at the Ouray, Utah site over January and February of the indicated ozone season. It indicates the importance of snow cover for ozone formation. For three seasons, 2012, 2015, and 2018, there was no snowpack, with av- erage snow depths never more than about 10 mm. By contrast, in the remaining seasons, 2010, 2011, 2013, 2014, 2016, 2017, 2019, and 2020, average snow depths were between about 80 and 240 mm. During each of the eight seasons with a snowpack, the ground was snow-covered for the entirety of January and February. Seasons without snow had average concentrations near the background value of about 40 ppb, while ozone concentrations during seasons with snow were always larger. All averages include contributions from Atmosphere 2021, 12, x FOR PEER REVIEW 5 of 19 both high and low ozone days. A p-test (Section 3.8) indicates that it is highly unlikely that the three low ozone seasons coincided with the three low snow seasons merely by chance.

FigureFigure 2. 2. SeasonalSeasonal average average of of the the daily daily maximum maximum in in the the 8-h 8-h running running average average ozone concentration at atOuray, Ouray, Utah Utah and and basin-average basin-average snow snow depth, depth, over over the the months months of of January January andand February,February, for for each eachof ofthe the 11 11 indicated indicated winter winter seasons. seasons.

3.2. Temporal Trends in Exceedance Counts Figure 3 displays the number of seasonal ozone exceedances attributable to the win- ter ozone phenomenon at Ouray, Utah, defined as the number of days for which the daily maximum in the eight-hour running average ozone concentration exceeded 70 ppb. With a Pearson’s R2 correlation coefficient of 0.77, ozone exceedances during seasons with snow have been declining at a rate of nearly four per season.

R2 = 0.77, slope = −3.8 ± 1.7 ance Count Ozone Exceed 0 1020304050 2009 2012 2015 2018 2021 Season

Figure 3. Seasonal ozone exceedances of the current National Ambient Air Quality Standard for ozone at the Ouray site. Seasons with and without snow cover are blue and red, respectively. The trend line for the seasons with snow cover is plotted and has the indicated slope and correlation coefficient.

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Atmosphere 2021, 12, 4 Figure 2. Seasonal average of the daily maximum in the 8-h running average ozone concentration5 of 18 at Ouray, Utah and basin-average snow depth, over the months of January and February, for each of the 11 indicated winter seasons.

3.2.3.2. Temporal Temporal Trends Trends in in Exceedance Exceedance Counts Counts FigureFigure 33 displays the number ofof seasonalseasonal ozoneozone exceedancesexceedances attributable attributable to to the the winter win- terozone ozone phenomenon phenomenon at at Ouray, Ouray, Utah, Utah, defined defined as as thethe numbernumber ofof days for which which the the daily daily maximummaximum in in the the eight-hour eight-hour ru runningnning average ozone concentration exceededexceeded 7070 ppb.ppb. WithWith a 2 aPearson’s Pearson’s RR2 correlation coefficient coefficient of 0.77, ozone ozone exceedances exceedances during during seasons seasons with with snow snow havehave been been declining declining at at a a rate rate of of nearly nearly four four per per season. season.

R2 = 0.77, slope = −3.8 ± 1.7 ance Count Ozone Exceed 0 1020304050 2009 2012 2015 2018 2021 Season

FigureFigure 3. 3. SeasonalSeasonal ozone ozone exceedances exceedances of the currentcurrent NationalNational Ambient Ambient Air Air Quality Quality Standard Standard for for ozone ozoneat the at Ouray the Ouray site. Seasons site. Seasons with and with without and without snow coversnow arecover blue are and blue red, and respectively. red, respectively. The trend The line trendfor the line seasons for the with seasons snow with cover snow is plotted cover is and plotted has the and indicated has the indicated slope and slope correlation and correlation coefficient. coefficient. 3.3. Correlations between Snow Depth and Pseudo-Lapse Rate As mentioned above, we calculate a quantity, Ψ, the daily pseudo-lapse rate, to char- acterize inversion strength. Figure4 demonstrates that the snowpack stabilizes and intensi- fies inversions. Atmosphere 2021, 12, x FOR PEER REVIEW 6 of 19

3.3. Correlations between Snow Depth and Pseudo-Lapse Rate Ψ Atmosphere 2021, 12, 4 As mentioned above, we calculate a quantity, , the daily pseudo-lapse rate, to 6char- of 18 acterize inversion strength. Figure 4 demonstrates that the snowpack stabilizes and inten- sifies inversions.

Seasons with snow

Seasons without snow Days withindicated the pseudo-lapse rate

-25 -20 -15 -10 -5 0 5 10 15 20 Pseudo-lapse rate, Ψ, K/km

FigureFigure 4. HistogramsHistograms of the distribution of the dailydaily pseudo-lapse rate,rate, distinguishingdistinguishing seasonsseasons with- withoutout snow snow (2012, (2012, 2015, 2015, 2018) 2018) from from seasons seasons with with snow snow (2010, (2010, 2011, 2011, 2013, 2013, 2014, 2014, 2016, 2016, 2017, 2017, 2019, 2019, 2020). 2020). 3.4. Correlations between Ozone Concentration and Pseudo-Lapse Rate 3.4. CorrelationsWe generated between scatter Ozone plots Concentration of daily ozone and concentrationPseudo-Lapse Rate vs. daily pseudo-lapse rate, resultingWe generated in 177 plots scatter when plots data of daily from ozone each season concentration and site vs are. daily considered pseudo-lapse separately. rate, resultingThe scatter in plots177 plots are foundwhen data in the from Supplementary each season and Material, site are while considered Figure 5separately. displays twoThe scatterexamples, plots selected are found for displayin the Supplementary because they have Material, among while the largest Figure correlation 5 displays coefficients,two exam- 2 ples,R . Theselected distributions for display of because the correlation they have coefficients among the and largest of the correlation site altitudes coefficients, across theR2. The177 distributions plots are shown of the in correlation Figure6. Many coefficients scatter and plots of dothe notsite havealtitudes an impressivelyacross the 177 large plots arecorrelation shown in coefficient, Figure 6. Many with some scatter near plots zero do and not nonehave largeran impressively than about large 0.7. correlation Because of coefficient,confounding with variables, some near e.g., zero solar and elevation none larger and snow than depth,about 0.7. large Because correlation of confounding coefficients should not be expected. Nevertheless, the scatter plots display an interesting pattern, summarized in Table1 and Figure6. In seasons when a snowpack is present, ozone concentrations and lapse rates are almost always negatively correlated (61% of all instances),

while they are almost always positively correlated when the snowpack does not form (34% of all instances). Only nine instances (5% of all) violate this pattern. Figure6 shows that Atmosphere 2021, 12, x FOR PEER REVIEW 7 of 19

variables, e.g., solar elevation and snow depth, large correlation coefficients should not be expected. Nevertheless, the scatter plots display an interesting pattern, summarized in Table 1 and Figure 6. In seasons when a snowpack is present, ozone concentrations and Atmosphere 2021, 12, 4 lapse rates are almost always negatively correlated (61% of all instances), while they7 ofare 18 almost always positively correlated when the snowpack does not form (34% of all in- stances). Only nine instances (5% of all) violate this pattern. Figure 6 shows that the pat- tern is more likely to be violated at high altitude sites and when the correlations are weak. the pattern is more likely to be violated at high altitude sites and when the correlations are Of the nine pairings that did not follow the pattern, six occurred at elevations above about weak. Of the nine pairings that did not follow the pattern, six occurred at elevations above 2000about m, 2000 or at m, sites or atabove sites the above inversion the inversion layer, and layer, all andhad allcorrelation had correlation coefficients coefficients below aboutbelow 0.15. about 0.15.

Roosevelt 2012 R2 = 0.607 Ouray 2014 R2 = 0.655 Ozone concentration, ppb

-924 28 -6 32 36 -3 40 44 0 48 52 3 6 9 12 -25 -15 -5 5 15 27 36 45 54 63 72 81 90 99 Pseudo-lapse rate, Ψ, K/km

FigureFigure 5. 5. WhenWhen a asnowpack snowpack is isabsent, absent, ozone ozone concentrat concentrationion and and pseudo-lapse pseudo-lapse rate rate at aat given a given site site areare almost almost always always positively positively correlated correlated (left). (left). When When a asnowpack snowpack is is present, present, they they are are almost almost always always negativelynegatively correlated correlated (right). (right). Least- Least-squaressquares trend trend lines lines are are shown shown in in blue. blue.

Table To1. The compare numbers variations of positive between or negative seasons, correla wetions plotted between on daily a single ozone graph concentration all the and trend dailylines pseudo-lapse from the ozone rate for vs. data lapse from rate any scatter one site plots in any from one season, any one when site. classified Figure 7by shows the sign the of theresultant correlation graph and forthe thepresence Ouray of site;a snow allpack, other follow such the plots distribution have similar shown appearance here. and are given in the Supplementary Material. A common feature is that the trend lines radiate outward from a convergencePositive zone Correlation (the blue Nega circle)tive characterized Correlation by neutral TOTALS lapse rates, Snowpack present 7 108 115 Ψ ≈ 9 K/km [27], and background ozone concentrations [O3] ≈ 40 ppb. During non-snow seasonsSnowpack (2012, absent 2015, 2018) the trend 60 lines usually radiate 2downward to the left, 62 while during snow seasonsTOTALS (2010, 2011, 2013, 2014,67 2016, 2017, 2019, 110 2020) they radiate upward. 177 In other words, non-snow seasons display ozone concentrations below background, which probably follows because inversions prevent background ozone from mixing in, and in the absence of adequate actinic flux, ozone titrates away faster than it is generated. But since the same mixing conditions occur when a snowpack is present, it probably also indicates that inversions during snow seasons also block out background ozone, implying that high ozone formation is local. Inexplicably, the 2010 trend line in Figure7 avoids the convergence zone; ozone in that season appears to be uncharacteristically high at positive or near-zero lapse rates. The 2010 trend line for Redwash behaves similarly (see the Supplementary Material), while no other 2010 data are available. This probably rules out equipment malfunction or other effects that could be attributed to a single site. The convergence zones for several high-altitude sites (Fruitland, Mountain Home, and Little Mountain, see the Supplementary Material) are shifted upwards to about 50 ppb. Figure7 shows a vertical red line at Ψ = −15 K/km. The point at which it intercepts each trend line defines the value h[O3]i−15. Think of h[O3]i−15 as the typical ozone concen- tration in any given season and at any given site when the pseudo-lapse rate is near −15 K/km. The horizontal red lines serve to identify the season to which each h[O3]i−15 value belongs, and by extension the season corresponding to each trend line. Atmosphere 2021, 12, 4 8 of 18 Atmosphere 2021, 12, x FOR PEER REVIEW 8 of 19

Figure 6. OutOut of of 177 177 available available pairings pairings of of measuremen measurementt sites sites and and measurement measurement seasons, seasons, the theover- over- whelming majority (gray and and green green bars) bars) fit fit a a pattern: pattern: Negative Negative correlation correlation between between ozone ozone con- concen- trationcentration and and lapse lapse rate rate (down (down arrows) arrows) when when snow snow is is present, present, andand positivepositive correlation (up (up ar- arrows) whenrows) snowwhen issnow not is present. not present. Only Only 5% of 5% the of 177 the instances177 instances (blue (blu ande and red red bars) bars) do notdo not fit thisfit this pattern. pattern. Two-thirds of the pattern violations occur at sites above about 2000 m (a) and all occur Two-thirds of the pattern violations occur at sites above about 2000 m (a) and all occur with small with small correlation coefficients (b). correlation coefficients (b). To compare variations between seasons, we plotted on a single graph all the trend lines from the ozone vs. lapse rate scatter plots from any one site. Figure 7 shows the re- sultant graph for the Ouray site; all other such plots have similar appearance and are given in the Supplementary Material. A common feature is that the trend lines radiate outward from a convergence zone (the blue circle) characterized by neutral lapse rates, Ψ≈

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9 TableK/km 1. [27],The numbersand background of positive orozone negative concentrations correlations betweenO ≈ 40 daily ppb ozone. During concentration non-snow and seasonsdaily pseudo-lapse (2012, 2015, rate 2018) for the data trend from anylines one usua sitelly in radiate any one downward season, when to classified the left, bywhile the signdur- of ingthe snow correlation seasons and (2010, the presence 2011, 2013, of a snowpack, 2014, 2016, follow 2017, the 2019, distribution 2020) they shown radiate here. upward. In other words, non-snow seasons display ozone concentrations below background, which probably follows becausePositive inversions Correlation prevent background Negative Correlation ozone from mixing TOTALS in, and in the absenceSnowpack of present adequate actinic flux, 7 ozone titrates away 108 faster than it is generated. 115 But sinceSnowpack the same absentmixing conditions 60occur when a snowpack 2 is present, it probably 62 also in- dicates thatTOTALS inversions during snow 67 seasons also block 110out background ozone, 177 implying that high ozone formation is local.

FigureFigure 7. 7.BlackBlack lines lines are are trend trend lines lines from from the the ozone ozone concentration concentration vs. vs. pseudo-lapse pseudo-lapse rate rate plots plots for for any anygiven given season season and and for for the the Ouray Oura site.y site. Usually, Usually, the the trend trend lines lines radiate radiate outward outward from from a a convergence conver- Ψ = −15 K/km genceregion region (vicinity (vicinity of the of blue the circle).blue circle). The vertical The vertical red line red at lineΨ = at− 15 K/km is used is to used define to hdefine[O3]i− 15, 〈i.e.,O〉 the, value i.e., the of eachvalue trend of each line trend when lineΨ = when−15 K/kmΨ = −15. Horizontal K/km. Horizontal red lines guidered lines the guide eye to the indicate eye tothe indicate corresponding the corresponding season. season.

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3.5. Interannual Trends in Ozone Concentration Figures2 and3 already provide evidence of the attenuation of ozone concentrations at the Ouray site. We now document this attenuation further, by examining the behavior of h[O3]i−15 at all sites and in all seasons. Figure8 shows box–whisker plots of the distribu- tions of h[O3]i−15 over all measurement sites in any given season. The difference between seasons with and without snow is obvious. The upper trend line suggests a gradual decline in ozone concentration of about 3 ppb each season over the decade. Figure8 also suggests an upward trend in h[O3]i−15 over the three seasons without snow. The downward trend in seasons with a snowpack appears to be statistically significant (Section 3.8). Statistical significance of the upward trend in seasons without snow cannot be established because of a lower statistical power. However, if both trends are assumed to be statistically significant, Atmosphere 2021, 12, x FOR PEER REVIEW 11 of 19 then they can be explained by a decline in NOx or other ozone precursors over the course of the decade. In the absence of adequate actinic flux, NOx titrates the ozone away.

FigureFigure 8. 8. Box–whiskerBox–whisker plots plots of the of thedistribution distribution of 〈 ofOh[〉O3]i − over15 over all sites all sitesin any in given any givenseason. season. WhiskersWhiskers extend extend from from the the minimum minimum to the to themaximu maximum;m; boxes boxes extend extend from fromthe 25th the to 25th the to75th the per- 75th centilepercentile with with medians medians also also shown. shown. Each Each box box is labe is labeledled with with the the number number of ofsites sites inin any any given given season. season. OnlyOnly two two datapoints datapoints are are available available in in 2010, 2010, so so a abo box–whiskerx–whisker construction construction is is not not possible. possible. Blue Blue and and red designate seasons with and without snow, respectively. The upper dashed line has slope = –3.0 red designate seasons with and without snow, respectively. The upper dashed line has slope = −3.0 ± 2.0 (95% confidence interval) ppb/season, and Pearson’s R2 = 0.61. It represents the trend line ± 2.0 (95% confidence interval) ppb/season, and Pearson’s R2 = 0.61. It represents the trend line drawn through the medians of seasons with snow. The lower dashed line (slope = +1.8 ppb/season, Rdrawn2 = 0.65) through is the trend the medians line for ofseasons seasons without with snow. snow. The lower dashed line (slope = +1.8 ppb/season, R2 = 0.65) is the trend line for seasons without snow. 3.6. Impact of Proximity to Well Pads Ten measurement sites provide data over all seasons from 2011 to 2019. Let 〈〈O〉〉 represent the average of 〈O〉 over the snow seasons between 2011 and 2019. It therefore represents the long-term average ozone concentration at any particular site when lapse rates are about –15 K/km and snow is on the ground. The local well density is defined as the number of well pads per km2 within a ten-kilometer radius of the meas- urement site. Figure 9 demonstrates that ozone concentrations are correlated with this local density. Proximity to well pads is a strong predictor of ozone concentration. The two outliers, Rabbit Mountain and Fruitland, lie at higher elevations, and can be expected to have lower ozone concentrations.

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3.6. Impact of Proximity to Well Pads hh[ ]i i Ten measurement sites provide data over all seasons from 2011 to 2019. Let O3 −15 S represent the average of h[O3]i−15 over the snow seasons between 2011 and 2019. It there- fore represents the long-term average ozone concentration at any particular site when lapse rates are about −15 K/km and snow is on the ground. The local well density is defined as the number of well pads per km2 within a ten-kilometer radius of the measurement site. Figure9 demonstrates that ozone concentrations are correlated with this local density. Atmosphere 2021, 12, x FOR PEER REVIEWProximity to well pads is a strong predictor of ozone concentration. The two outliers,12 of 19 Rabbit Mountain and Fruitland, lie at higher elevations, and can be expected to have lower ozone concentrations.

hh[ ]i i FigureFigure 9. 9. PlotPlot of of 〈〈OO3〉−15〉, Srepresenting, representing the the long-term long-term aver averageage ozone ozone concentration concentration when when the the lapselapse rate rate is is caca.. −−1515 K/km K/km and and when when a asnowpack snowpack is is present, present, vs. vs. local local well density atat tenten measurementmeasure- mentsites. sites. Numbers Numbers in parenthesesin parentheses are are the the elevations elevations (m) (m) of of each each site. site. TheThe red trace trace is is a a suggested suggested correlationcorrelation curve. curve.

3.7.3.7. Interannual Interannual Trends Trends in in Ozone Ozone Precursor Precursor Concentrations Concentrations DownwardDownward trends trends in in ozone ozone precursor precursor emissions emissions and and concentrations concentrations are are the the most most likelylikely explanation explanation for for the the downward downward trend trend in inozone. ozone. This This section section presents presents an ananalysis analysis of interannualof interannual trends trends in winter in winter season-average season-average ozone ozone precursor precursor concentrations. concentrations. We used We used the seasonthe season averages averages of (1) of all (1) available all available data, data,(2) data (2) datafrom fromdays dayswhen when the pseudo-lapse the pseudo-lapse rate wasrate above was above zero (to zero eliminate (to eliminate bias caused bias caused by precursor by precursor buildup buildup during during inversion inversion epi- sodes),episodes), and and(3) precursor (3) precursor concentrations concentrations multip multipliedlied by wind by wind speed speed (to account (to account for the for ef- the fectseffects of ofwind wind speed speed on on concentrations) concentrations) on on days days when when the the pseudo-lapse pseudo-lapse rate rate was was above above zero.zero. All All three three methods methods showed showed similar similar interannual interannual trends, trends, but but method method 2 2 resulted resulted in in less less interannualinterannual variability variability (i.e., (i.e., smoother smoother trends). trends). We We present present the the results results of of method method 2 2 here. here. Figure 10 shows the seasonal average NOx concentrations at all sites with available Figure 10 shows the seasonal average NOx concentrations at all sites with available data along with medians for each season. The mean of the medians over the last four data along with medians for each season. The mean of the medians over the last four sea- seasons (2017–2020) is only 58% of the mean over the first four seasons (2010–2013). The four sons (2017–2020) is only 58% of the mean over the first four seasons (2010–2013). The four highest medians occurred in the first four years, 2010–2013. At all sites but Whiterocks highest medians occurred in the first four years, 2010–2013. At all sites but Whiterocks and Vernal, the averages over 2017–2020 are between 42% and 74% of averages over 2010– and Vernal, the averages over 2017–2020 are between 42% and 74% of averages over 2010– 2013. Vernal saw an even larger decline to 38%, probably because the Vernal monitoring 2013. Vernal saw an even larger decline to 38%, probably because the Vernal monitoring station moved in 2015 to a site more removed from possible NOx sources (from near a station moved in 2015 to a site more removed from possible NOx sources (from near a busy highway and airport to the edge of the metropolitan area). Whiterocks saw a decline busy highway and airport to the edge of the metropolitan area). Whiterocks saw a decline to only 91%, but NOx there is consistently low. The correlation between NOx and time to only 91%, but NOx there is consistently low. The correlation between NOx and time is negative at all sites. The trend line through the medians has slope –0.32 ± 0.10 (95% confi- dence interval) ppb/season and Pearson’s R2 = 0.79.

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Atmosphere 2021, 12, x FOR PEER REVIEW 13 of 19 is negative at all sites. The trend line through the medians has slope −0.32 ± 0.10 (95% confidence interval) ppb/season and Pearson’s R2 = 0.79.

FigureFigure 10. 10. WinterWinter season season average average NO NOx fromx from Uinta Uinta Basin Basin monitoring monitoring stations. stations. Only data Only from data days from withdays a withpseudo-lapse a pseudo-lapse rate above rate zero above are zero included are included.. Data shown Data are shown the average are the of average each site. of eachThe site. mediansThe medians taken takenover all over sites all in sites each in single each single season season and the and trend the trendline through line through these thesemedians medians are are alsoalso shown. shown. The The trace trace for for Vernal Vernal is is broken broken beca becauseuse the the monitoring monitoring site site moved moved in in 2015 2015 to to a a site site more more distant from possible NOx sources. distant from possible NOx sources.

OrganicOrganic compound compound data data have have only only consiste consistentlyntly been been collected collected at at the the Horsepool Horsepool and and RooseveltRoosevelt sites. sites. The The collection andand analysisanalysismethods methods changed changed over over time, time, with with real-time real-time GC GCthrough through 2015, 2015, and and three-hour three-hour once-daily once-daily (beginning (beginning at at midnight midnight or or noon noon MST) MST) whole-air whole- aircanister canister samples samples thereafter. thereafter. Figure Figure 11 11 showsshows thatthat average concentrations concentrations of of total total non- non- methanemethane hydrocarbons hydrocarbons (TNMHC), ethane,ethane, and and toluene toluene have have all all declined declined since since 2012 2012 or 2013, or 2013,but havebut have rebounded rebounded in recent in recent years. years. TNMHC TNMHC and and ethane ethane in Roosevelt in Roosevelt declined declined in 2018 in 2018to about to about 20% 20% to 50% to of50% the of initial the initial 2013 value,2013 value, and then and reboundedthen rebounded to about to about 50% to 50% 90% to in 90% in 2020. At Horsepool, TNMHC and ethane declined in 2018 and 2019 to about 30% to 50% of the 2012 value, and then recovered to about 50% to 90% in 2020. Toluene was

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Atmosphere 2021, 12, x FOR PEER REVIEW 14 of 19

2020. At Horsepool, TNMHC and ethane declined in 2018 and 2019 to about 30% to 50% of the 2012 value, and then recovered to about 50% to 90% in 2020. Toluene was present at presentboth sites at atboth concentrations sites at concentrations of only about of 1–2only ppb. about It also 1–2 passedppb. It through also passed a minimum through and a minimumthen rebounded and then to aboutrebounded 85% toto 165%about of 85% the to 2012 165% or 2013of the value. 2012 or 2013 value. Roosevelt Horsepool

+0.23 +0.25 0.68−0.19 0.73−0.22 TNMHC, ppb TNMHC,

+0.13 +0.08 0.32−0.11 0.42−0.08 0 100 200 300 400

+0.25 +0.24 0.71−0.21 0.67−0.21 Ethane, ppb

+0.15 +0.14 0.34−0.13 0.41−0.12 0 20406080100120

+0.38 +0.45 1.30−0.35 1.20−0.40 Toluene, ppb

+0.06 +0.28 0.50−0.05 0.54−0.18 0.0 0.5 1.0 1.5 2.0 2.5 3.0 2012 2014 2016 2018 2020 2012 2014 2016 2018 2020

FigureFigure 11. 11. Time-lineTime-line plots plots of of the the average average winter-time winter-time concentrations concentrations of TN of TNMHC,MHC, ethane, ethane, and and toluene. toluene. Whiskers Whiskers show show the 95%the 95%bootstrap bootstrap confidence confidence intervals intervals of each of each mean. mean. Selected Selected datapoints datapoints are arelabeled labeled in inred red with with the the ratio ratio of of the the mean mean concentrationconcentration in in the the indicated indicated season season to to the the mean mean concentration concentration in in the the initial initial seas season;on; subscripts subscripts and and superscripts superscripts give give the the limitslimits of of the the 95% 95% bootstrap bootstrap confidence confidence intervals intervals of of each each ratio. ratio.

3.8.3.8. Tests Tests of of Statistical Statistical Significance Significance OneOne test test of of statistical statistical significancesignificance ofof timelinetimeline trends trends is is to to calculate calculate confidence confidence intervals inter- valsfor thefor slopes.the slopes. Table Table2 summarizes 2 summarizes results results for the for trendthe trend lines lines in Figures in Figures3,8 and 3, 8,10 and. Zero 10. Zeroslope slope lies outside lies outside the confidence the confidence intervals, interval indicatings, indicating that all that three all slopes three are slopes non-zero are non- with zerobetter with than better 95% than confidence. 95% confidence.

Table 2. 95% confidence intervals for the slopes of several trend lines.

Trend Line Slope with Confidence Interval Ozone exceedance count, Figure 3 −3.8 ± 1.7 counts per year ± 〈O〉, Figure 8 −3.0 2.0 ppb per year NOx medians, Figure 10 −0.32 ± 0.10 ppb per year

Atmosphere 2021, 12, 4 14 of 18

Table 2. 95% confidence intervals for the slopes of several trend lines.

Trend Line Slope with Confidence Interval Ozone exceedance count, Figure3 −3.8 ± 1.7 counts per year h[O3]i−15, Figure8 −3.0 ± 2.0 ppb per year NOx medians, Figure 10 −0.32 ± 0.10 ppb per year

Table3 summarizes several p-tests that have been applied to the data. p represents the probability that the indicated occurrence or null hypothesis could have occurred randomly. For the first three occurrences, p is determined by combinatorics. For the remaining two, p was determined by Monte Carlo calculations in which we scrambled the x-coordinates of all points, and then computed the probability that any least-squares line is at least as steep as the line through the unscrambled data. The p values are all much lower than the threshold, 0.05, traditionally cited as the indicator for statistical significance. They all indicate that the trends observed in Figures2,3,8 and 10 are statistically significant.

Table 3. Results of tests of statistical significance: The probability that the indicated occurrence could have occurred at random.

OCCURENCE p 3!8! ∼ Three seasons with no snow out of 11 total were the same three seasons to have low ozone, Figure2. 11! = 0.006 Figures2,3 and8 all display some metric of ozone levels; the three largest values of the metric occur in 3!5! =∼ 0.018 the first three out of eight snow seasons. 8! 4!7! ∼ The first four NOx seasons out of 11 total were the same to display the four largest medians, Figure 10. 11! = 0.003 The medians over the eight snow seasons in Figure8 are sufficiently ordered to trend downward at least =∼ 0.015 as steeply as −3 ppb/year. The medians over the 11 seasons in Figure 10 are sufficiently ordered to trend downward at least as =∼ 0.0003 steeply as −0.325 ppb/year.

3.9. Trends in the Oil and Natural Gas Industry The data indicate that winter ozone in the Uinta Basin has been declining since it was first measured in 2010. There are probably two causes for the decline: (1) a decrease in global demand for oil and natural gas has led to decreased industrial activity; and (2) many pollution controls have come online over the last decade. At the time of writing this, we have no way of knowing the relative importance of either cause. Global market forces drive fossil fuel production. Price increases led to an increase in drilling [28], wells, and oil and gas production in the Uinta Basin until 2014 [26] (Figure 12). A price collapse after 2014 caused a rapid decline in drilling, which led to a leveling-off and then a slow decline in the number of producing wells in the Basin. Oil production peaked in 2015 and, after a drop in 2016 and 2017, has been steady at about 375 million L/month from 2018 through 2020, 70% higher than the 2010–2012 average. Gas production has steadily declined from a peak of about 8 × 108m3/month in 2010–2012 to only 64% of that in 2018–2020. Atmosphere 2021, 12, x FOR PEER REVIEW 15 of 19

Table 3 summarizes several p-tests that have been applied to the data. p represents the probability that the indicated occurrence or null hypothesis could have occurred ran- domly. For the first three occurrences, p is determined by combinatorics. For the remain- ing two, p was determined by Monte Carlo calculations in which we scrambled the x- coordinates of all points, and then computed the probability that any least-squares line is at least as steep as the line through the unscrambled data. The p values are all much lower than the threshold, 0.05, traditionally cited as the indicator for statistical significance. They all indicate that the trends observed in Figures 2, 3, 8, and 10 are statistically significant.

Table 3. Results of tests of statistical significance: The probability that the indicated occurrence could have occurred at random.

OCCURENCE p Three seasons with no snow out of 11 total were the same three seasons to have low 3! 8! ≅ 0.006 ozone, Figure 2. 11! Figures 2, 3, and 8 all display some metric of ozone levels; the three largest values of 3! 5! ≅ 0.018 the metric occur in the first three out of eight snow seasons. 8! The first four NOx seasons out of 11 total were the same to display the four largest 4! 7! ≅ 0.003 medians, Figure 10. 11! The medians over the eight snow seasons in Figure 8 are sufficiently ordered to trend ≅ 0.015 downward at least as steeply as −3 ppb/year. The medians over the 11 seasons in Figure 10 are sufficiently ordered to trend ≅ 0.0003 downward at least as steeply as −0.325 ppb/year.

3.9. Trends in the Oil and Natural Gas Industry The data indicate that winter ozone in the Uinta Basin has been declining since it was first measured in 2010. There are probably two causes for the decline: (1) a decrease in global demand for oil and natural gas has led to decreased industrial activity; and (2) many pollution controls have come online over the last decade. At the time of writing this, we have no way of knowing the relative importance of either cause. Global market forces drive fossil fuel production. Price increases led to an increase in drilling [28], wells, and oil and gas production in the Uinta Basin until 2014 [26] (Figure 12). A price collapse after 2014 caused a rapid decline in drilling, which led to a leveling- off and then a slow decline in the number of producing wells in the Basin. Oil production peaked in 2015 and, after a drop in 2016 and 2017, has been steady at about 375 million Atmosphere 2021, 12, 4 L/month from 2018 through 2020, 70% higher than the 2010–2012 average. Gas production15 of 18 has steadily declined from a peak of about 8 10 m⁄month in 2010–2012 to only 64% of that in 2018–2020.

Figure 12. Number of producing oil and gas wells, total natural gas production, and total oil production in the Uinta Basin for the month of February of the indicated season. Average number of drilling rigs in the state of Utah each February is also shown.

Drilling is an important source of NOx, while the production of oil and gas is linked to both NOx and organic emissions. The data suggest that the decline in ozone precursor concentrations may be linked in part to the declines in drilling or to gas production.

3.10. Pollution Controls Pollution controls at oil and gas wells, either mandated by government regulation or installed voluntarily by owners, have increased over the last decade. In 2012 the U.S. Environmental Protection Agency (EPA) issued Code of Federal Regulations (CFR) 40, Part 60, Subpart OOOO (a.k.a., Quad-O), which regulates organic compound emissions from oil and gas facilities [29–31]. It was implemented in a phased approach between October 2012 and October 2015. Quad-O regulations only apply to facilities constructed or modified after the implementation dates. In total, 85% of oil and gas wells in the Uinta Basin were completed before October 2013, when the first of the Quad-O provisions that affect well-site operations took effect. Seventy-seven percent of the wells completed since October 2013 are oil wells. EPA issued a separate rule in 2012 restricting emissions of hazardous air pollutants from glycol dehydrators to a total of less than 25 tons/year [29,30]. This rule applied to new and existing dehydrators, and was phased in between 2012 and 2015. An emissions inventory developed by the Utah Division of Air Quality for the year 2014 showed that, of 1904 glycol dehydrators in the Uinta Basin, only 0.2% had emissions of total volatile organics greater than 25 tons/year [32]. Thus, we assume this rule had a small impact on emissions of ozone-forming organics in the Uinta Basin. Additional regulation promulgated by EPA in 2016 (CFR 40, Part 60, Subpart OOOOa; a.k.a., Quad-Oa) requires companies that construct new oil and gas facilities to inspect those facilities for natural gas leaks periodically (usually semiannually), and to repair leaks that are found [31]. Even though Quad-Oa only applies to new or modified facilities, in a survey of Uinta Basin oil and gas producers conducted in 2018 by Lyman et al. [33], 83% of respondents indicated they inspected all oil and gas wells at least annually. The same study showed that when one company implemented a leak detection and repair program that was more aggressive than EPA requirements, along with upgraded emissions control equipment, detection of emission plumes at that company’s wells dropped by 79%. The Utah Division of Air Quality has also adopted standards to control organic compound emissions from oil and gas wells [34]. These standards are either the same as, or similar to, Quad-O and Quad-Oa regulations. Atmosphere 2021, 12, 4 16 of 18

4. Discussion and Conclusions At neutral atmospheric conditions, Ψ ≈ 9 K/km [27], ozone tends to be near the background value of about 40 ppb, during seasons both with and without snowpacks. Under inversion conditions, Ψ ≈ −15 K/km, and when a snowpack is present, ozone concentrations are above background, depend on proximity to oil and gas wells, and de- crease over time. Under inversion conditions, Ψ ≈ −15 K/km, and in the absence of a snowpack, ozone concentrations are below background and appear to be increasing over time. The most logical explanation is that compounds responsible for ozone production when the actinic flux is high (NOx and organics), and for ozone reduction when the actinic flux is low (NOx), have been decreasing. Indeed, trends in ozone precursors have paralleled the decrease in ozone over the previous decade. Ozone and NOx concentrations at all sites have been trending down at the rate of about 3 and 0.3 ppb/year, respectively. Average ozone concentrations over the three-year period 2017, 2019, and 2020 are only about 67% of the concentrations over the period 2010, 2011, and 2013. Average NOx concentrations over the period 2018–2020 are 58% of those over 2010–2012. Average concentrations of organics fell in 2018 to about 40% of their 2012 or 2013 values. The concentration of organics has shown an upturn in recent years, due perhaps to new sources that have come online recently. Several p-tests indicate that the declines in ozone and NOx are statistically significant. Several years ago, we drew comparisons between the Uinta Basin of Utah and the Upper Green River and Wind River Basins of Wyoming [9]. All three basins experience persistent inversions, snowpacks, and are home to oil or natural gas extraction. The Upper Green and the Wind River Basins are at comparable latitudes and therefore see the same solar elevation. However, high winter ozone occurs in the Uinta and Upper Green River Basins, but not in the Wind River Basin, presumably because oil or gas production there is lower. This suggests that there is a threshold for oil and gas emissions above which high ozone begins to occur, but below which ozone remains at background levels. The two trend lines in Figure8 are converging, indicating that the Uinta Basin may be approaching that threshold. A number of authors have presented evidence that the Uinta Basin ozone system is NOx-limited [17,35]. Insensitivity to the recent upturn in organics emissions may also be an indication of NOx control. We believe that there are two causes for the decrease in ozone precursor concentrations. First, declines in the global demand for oil and natural gas have led to a decrease in oil and gas extraction activity. Second, government-mandated and voluntary pollution controls have come online since 2010 (Section 3.10). However, these controls only targeted emissions of organics. They cannot explain the decline in NOx concentrations. The trends in well- drilling or gas production documented in Figure 12 may explain the NOx decline. The trend line in Figure3 reaches zero exceedance days per season in 2020. The trend line in Figure8 has been below 70 ppb since 2014, and is converging on background ozone levels. These are encouraging trends, but there could very well be a resurgence of winter ozone if fossil fuel extraction activity increases in the Basin.

Supplementary Materials: The following are available online at https://www.mdpi.com/2073-443 3/12/1/4/s1, Winter Ozone Pollution in Utah’s Uinta Basin is Attenuating. Author Contributions: Conceptualization, M.L.M. and S.N.L.; methodology, M.L.M. and S.N.L.; validation, S.N.L.; formal analysis, M.L.M. and S.N.L.; investigation, M.L.M. and S.N.L.; data curation, S.N.L.; writing—original draft preparation, M.L.M. and S.N.L.; writing—review and editing, M.L.M. and S.N.L.; project administration, S.N.L.; funding acquisition, S.N.L. All authors have read and agreed to the published version of the manuscript. Funding: This research was funded by the Uintah County Impact Mitigation Special Services District and by the Legislature of the State of Utah. Conflicts of Interest: The authors declare no conflict of interest. Atmosphere 2021, 12, 4 17 of 18

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28. Baker-Hughes, North America Rig Count. Available online: https://bakerhughesrigcount.gcs-web.com/na-rigcount?c=79687& p=irolreportsother%20%3erigs%20by%20state%20current%20and%20historical%20%20this%20is%20the%20rig%20count%20for% 20the%20whole%20state (accessed on 12 October 2020). 29. Carbonell, T. EPA Issues Final Emission Standards for Oil and Gas Sector. 2012. Available online: https://www.vnf.com/ webfiles/VNF_Alert_4-20-12.pdf (accessed on 12 October 2020). 30. Healey, B.; Pergande, K. Breaking down Quad-O regulations, compliance needs. Pipeline Gas J. 2014, 241, 90–94. 31. Federal Register, Environmental Protection Agency. Oil and Natural Gas Sector: Emission Standards for New, Reconstructed, and Modified Sources. Available online: https://www.gpo.gov/fdsys/pkg/FR-2016-06-03/pdf/2016-11971.pdf (accessed on 14 October 2020). 32. Utah Division of Air Quality, 2014 Air Agencies Oil and Gas Emissions Inventory: Uinta Basin. Available online: https: //deq.utah.gov/air-quality/2014-air-agencies-oil-and-gas-emissions-inventory-uinta-basin (accessed on 18 October 2020). 33. Lyman, S.N.; Tran, T.; Mansfield, M.L.; Ravikumar, A.P. Aerial and ground-based optical gas imaging survey of Uinta Basin oil and gas wells. Elem. Sci. Anth. 2019, 7, 43. [CrossRef] 34. Utah Division of Air Quality, Centralized Air Emissions Reporting System. Available online: https://deq.utah.gov/air-quality/ centralized-air-emissions-reporting-system (accessed on 12 October 2020). 35. Womack, C.C.; McDuffie, E.E.; Edwards, P.M.; Bares, R.; de Gouw, J.A.; Docherty, K.S.; Dubé, W.P.; Fibiger, D.L.; Franchin, A.; Gilman, J.B.; et al. An Odd Oxygen Framework for Wintertime Ammonium Nitrate Aerosol Pollution in Urban Areas: NOx and VOC Control as Mitigation Strategies, Geophysical Research Letters. Soil Water Clim. 2019, 46, 4971–4979.