3.2. Evaluation and Comparison of Air Pollutants Concentrations
A comparison of the air pollutant concentrations at the investigated sites and times indicated their differences among the residential, traffic, and work sites during the selected study periods. The CD method of comparison was applied to the concentrations of air pollutants, and the resultant values described the degree of similarity between the two sites. Similar sites had CD values approaching zero, whereas different sites had CD values approaching one.
Figure 2 and
Table S3 show the degree of similarity or discrepancy in the air pollutant concentrations among the selected residential, traffic, and work sites during the selected study periods. Generally, the highest dissimilarity was observed for NO
x with a CD value of 0.66, followed by CO and SO
2 with CD values of 0.61 and 0.60, respectively. In contrast, low discrepancy or high similarity was observed for PM
10 and PM
2.5 concentrations during all investigated periods with CD values ranging from as low as 0.04 and up to 0.34 (
Figure 2 and
Table S3).
In a pairwise comparison of the unrestricted periods, the highest dissimilarity between residential and traffic sites was indicated by a divergence value of 0.43 for NO, whereas the highest dissimilarity between residential and work sites was indicated by divergence value of 0.60 for SO
2, and that between traffic and work sites was indicated by divergence value of 0.66 for NO
x (
Figure 2 and
Table S3). In contrast, the least discrepancy, and thus the highest similarity, was observed between residential and work sites (divergence value of 0.12) for NO, followed by that between residential and traffic sites (divergence ratio of 0.17) for NO
2 and that between residential and traffic sites (divergence value of 0.21) for CO (
Figure 2 and
Table S3). The discrepancy in CO and NO
2 pollutants between traffic and work sites (divergence ratios of 0.56 and 0.57, respectively) and between residential and work sites (divergence values of 0.40 and 0.56, respectively) exceeded the discrepancy in CO and NO
2 pollutants between residential and traffic sites (divergence values of 0.21 and 0.17, respectively) (
Figure 2 and
Table S3). Therefore, in terms of CO and NO
2 concentrations during the unrestricted periods, sites more similar and dissimilar to the residential site (M-station) were the traffic site (F-station) and work site (K-station), respectively.
In a pairwise comparison of the lockdown period, the highest dissimilarity between residential and traffic sites was indicated by a divergence value of 0.46 for NO, while the highest dissimilarity between residential and work sites was indicated by a divergence value of 0.57 for SO
2, and that between traffic and work sites was indicated by a divergence value of 0.61 for CO (
Figure 2 and
Table S3). In contrast, the least discrepancy, and thus the highest similarity, was observed between the residential and work sites (divergence ratio of 0.04) for PM
2.5, followed by that between the traffic and work sites (divergence value of 0.09) for PM
2.5 and that between the residential and traffic sites (divergence value of 0.20) for CO (
Figure 2 and
Table S3). The discrepancy in CO and NO
2 pollutants between the traffic and work sites (divergence values of 0.61 and 0.46, respectively) and between the residential and work sites (divergence values of 0.50 and 0.53, respectively) exceeded the discrepancy in CO and NO
2 pollutants between the residential and traffic sites (divergence values of 0.20 and 0.33, respectively) (
Figure 2 and
Table S3). Therefore, in terms of CO and NO
2 concentrations during the lockdown period, sites more similar and dissimilar to the residential site (M-station) were the traffic site (F-station) and work site (K-station), respectively. Moreover,
Figure 2 and
Table S2 also indicate that the lockdown decreased the range of CD values describing the similarity and discrepancy degrees among the three sites in terms of NO, NO
2, and NO
x, while the lockdown increased the range of CD values in terms of CO. The range of CD values in terms of NO, NO
2, and NO
x decreased by 185% (from 0.12–0.49 to 0.36–0.49), 100% (from 0.17–0.57 to 0.33–0.53), and 207% (from 0.23–0.66 to 0.39–0.53), respectively. In contrast, the range of CD values in terms of CO increased by 15% (from 0.21–0.56 to 0.20–0.61).
3.3. Comparison of the Selected Periods
To evaluate the effect of the lockdown on air quality, the measured concentrations of air pollutants for two of the three studied sites (residential M-station and traffic F-station) during the lockdown (denoted by M-20 and F-20 for the residential and traffic sites, respectively) were compared with those recorded during two selected periods. The first period of these was the corresponding period of the lockdown in 2019 (denoted by M-19 and F-19 for the residential and traffic sites, respectively), and the second period was the 22 days before the lockdown in 2020 (denoted by M-pre-20 and F-pre-20 for the residential and traffic sites, respectively). For the work site (K-station), the measured concentrations of air pollutants during the lockdown (K-20) were compared only with those measured during the 22 days after the lockdown in 2020 (K-post) because of the unavailability of recorded data in 2019 and pre-lockdown in 2020.
Figure 3 depicts a boxplot comparison of the hourly concentrations of air pollutants, including CO, NO, NO
2, NO
x, SO
2, O
3, and daily concentrations of particulate matter (PM
2.5 and PM
10). Generally, the interquartile ranges of most investigated gaseous air pollutants were wider for the traffic site than for the residential and work sites. All sites experienced significant decreases in the concentration levels of gaseous air pollutants during the lockdown period, except for SO
2 at the residential site and O
3 at the work site, both of which increased (
Figure 3 and
Figure 4). An increase in O
3 concentrations was observed during the lockdown in many countries around the world [
19,
20,
21,
22,
23]. In the three studied sites, the lockdown period compared with other periods also had the lowest median and mean concentration values of the investigated gaseous air pollutants, except for SO
2 in the residential site and O
3 at the work site (
Figure 3). Moreover, the maximum outlier values of gaseous air pollutants were higher at traffic sites than at residential and work sites but generally were approximately comparable for PM
10 and PM
2.5 at all three sites (
Figure 3). The PM
10 and PM
2.5 concentration changes were predominantly controlled by the frequent dust storms affecting the city; thus, the lockdown had only a slight effect on their concentration levels.
The percent changes in the concentrations of air pollutants at each station during the lockdown period are shown in
Figure 4. The greatest decrease during lockdown was observed in the NO concentrations at all three sites. The residential and traffic sites experienced the highest decrease in the concentration levels of NO, NO
x, and NO
2, while the work site had the lowest decreases in concentration levels of air pollutants. Furthermore, the residential and work sites exhibited similar decreasing profiles (NO > NO
x > NO
2 > CO). Comparing pollutant concentrations of the lockdown period with those of the corresponding period in 2019 and to the pre-lockdown period in 2020, the traffic site had comparable decreases in concentration levels of gaseous air pollutants, while the residential site exhibited comparable decreases only in concentration levels of NO
x and NO
2. At this residential site, NO and CO had different decreases in concentration levels whereas SO
2 increased in concentration during the lockdown period relative to the pre-lockdown period in 2020 but not with respect to the period in 2019. This indicated that the residential site experienced specific activities in 2019 (presumably construction activities), resulting in higher ambient concentrations of SO
2 than those recorded during the lockdown period. The observed increase in SO
2 concentration at the residential site during the lockdown relative to those of the pre-lockdown period in 2020 might be due to increased activities of heavy-duty diesel engines associated with construction activities near the site. However, this increase in construction activities was less than that in 2019. However, comparing PM
10 concentrations during the lockdown period with those during the corresponding period in 2019 at the traffic site revealed a decrease of ~22% in PM
10 concentrations during the lockdown, while the same comparison at the residential site increased by ~2% in PM
10 concentrations during the lockdown. Assuming similar PM
10 concentrations at the two sites resulting from dust storms affecting the city, this probably indicated that the residential site had additional emission sources of PM
10 other than dust storms. In addition to this increase in PM
10 at the residential site, no increases in pollutant concentrations were observed at the residential and traffic sites when the pollutant concentrations of the lockdown period were compared with those of the corresponding period in 2019. At the work site, the observed O
3 concentration increase during the lockdown was due to the observed declining NO
x concentration levels and evidence of a hydrocarbon-limited regime in Riyadh, as previously reported [
24]. In such a regime, the O
3 production rate is limited by the supply of hydrocarbons, and O
3 concentrations increase with increasing hydrocarbons and decrease with increasing NO
x [
25,
26,
27].
Figure 5 shows the diurnal distribution of average hourly O
3 and NO
x concentrations and their correlations during and after the lockdown at the work site (K-station). A typical systematic pattern of diurnal O
3 change is characterized by a daytime high and nighttime low. This pattern was observed only during the period after the lockdown ended. Both periods (during and after the lockdown) had typical daytime maxima. However, during the lockdown period, the minima were at daytime rather than nighttime (
Figure 5a,b). Following the diurnal variation in solar radiation, the O
3 concentration increased gradually after sunrise and reached its highest concentration of ∼67 ppb at 14:00 during the lockdown and ∼75 ppb at 10:00–12:00 during the period after the lockdown and gradually declined thereafter (
Figure 5a,b). The O
3 concentration decreased to its lowest value of ∼32 ppb at 7:00 (after sunrise) during the lockdown and to ∼22 ppb at 5:00 (before sunrise) during the period after the lockdown (
Figure 5a,b). Moreover, the nighttime O
3 concentration during the lockdown period (ranging from 34.1 to 47.3 ppb) was higher than the nighttime O
3 concentration during the period after the lockdown (ranging from 22.4 to 34.6 ppb). In addition,
Figure 5c,d shows the diurnal patterns of NO
x corresponding to the same two periods. The anticorrelation between O
3 and NO
x (R
2 = 0.59) during the period after the lockdown is clearly illustrated by comparing
Figure 5b,d,f, whereas this anticorrelation did not exist (R
2 = ~0) during the lockdown period (
Figure 5a,c,e). Furthermore, these same figures show that the NO
x concentration during the lockdown period lay in the range of 18.8–30.2 ppb during daytime (~6:00–19:00) and in the range of 17.6–24.5 ppb during nighttime. In contrast, the NO
x concentration during the period after the lockdown lay in the range of 6.9–51 ppb during the daytime and in the range of 27.3–57.7 ppb during nighttime. The reactions of NO with O
3 (NO + O
3 → NO
2 + O
2) and NO
2 with O
3 (NO
2 + O
3 → NO
3 + O
2) control the nighttime O
3 concentration [
28,
29]. Therefore, the relatively lower nighttime NO
x concentration during the lockdown period compared with those during the period after the lockdown indicated lower O
3 depletion by NO
x and explained the relatively higher nighttime O
3 concentration during the lockdown period. Finally, the distribution of the hourly average O
3 concentrations observed during the two periods is shown in
Figure 5g,h. In these figures, hourly O
3 concentrations are placed into predetermined 20 ppb bins. A maximum frequency value at O
3 concentrations of 40–60 ppb was observed during both periods. However, O
3 concentrations during the lockdown period followed a distribution that resembled a normal distribution to an extent, while those during the period after the lockdown exhibited a skewed distribution with a peak to the left (i.e., at low values) and a tail to the right (i.e., at high values). This type of skewed distribution indicated that anthropogenic pollution, particularly road traffic emissions, had a significant effect on the O
3 concentrations observed during the period after the lockdown.
3.4. Analysis of Exceedances and Air Quality Index for Individual Pollutants
For evaluation and comparison, we calculated air pollutant exceedances and AQIs. At the three studied sites, the air pollutant exceedances during the lockdown period were calculated based on the General Authority for Meteorology and Environmental Protection (GAMEP) and USEPA standards (
Table S4). The AQIs in this study were calculated using the USEPA standard formulae and air quality standard limits, as stated in the Materials and Methods section. Air quality data covering the corresponding lockdown period in 2019, the pre-lockdown period in 2020, and the lockdown and post-lockdown periods were used to calculate the index values. PM
10 and PM
2.5 were averaged daily, and O
3 was averaged every 1 and 8 h to match the breakpoint. The AQIs for individual pollutants during the selected periods are listed in
Table 1. No hourly exceedances for CO, NO
2, and SO
2; daily exceedances for SO
2; and 8 h exceedances for CO were observed in all stations during the entire lockdown period (
Table 2). Similarly, the AQI for CO and SO
2 had 0% undesired air at all stations during the lockdown (
Table 1). However, the AQI for hourly NO
2 concentrations revealed 0.7%, 1.06%, and 0.61% undesired air quality at the residential, traffic, and work sites, respectively, during the lockdown (
Table 1). In contrast, the AQI for hourly NO
2 concentrations had 6.99% undesired air quality during the corresponding lockdown period in 2019 and 4.39% undesired air quality during the pre-lockdown period in 2020 at the residential site. Similarly, the AQI for hourly NO
2 concentrations had 6.99% undesired air quality during the corresponding lockdown period in 2019 and 3.74% undesired air quality during the pre-lockdown period in 2020 at the traffic site, while the AQI for hourly NO
2 concentrations had 1.83% undesired air quality during the post-lockdown period at the work site. The percentages of undesired air quality reflected a good improvement in air quality in terms of NO
2 at their respective sites during the lockdown since the other investigated periods (the corresponding lockdown period in 2019, pre-lockdown period in 2020, and post-lockdown period) experienced higher percentages of undesired air quality at these sites (
Table 1).
For O
3, the 8 h O
3 concentration exceeded GAMEP and USEPA standards by 78 and 113 times, respectively, at the work site; 1 h O
3 concentrations at the work site exceeded both GAMEP and USEPA standards by two times. At the work site, the lockdown period was better in compliance with the 1 h O
3 standard than with the 8 h O
3 standard. The 8 h GAMEP standard and USEPA standard were exceeded 39 and 66.5 times, respectively, more often than the 1 h standard during the lockdown period (
Table 2). For human health, the 8 h O
3 standard provides better protection than the 1 h standard. According to hourly AQI, the lockdown period had less undesirable air (0.05%) than the K-post 20. In contrast, based on the 8 h AQI, K-post 20 had less undesirable air (32.56%) than during the lockdown period. Therefore, exposure times longer than 1 h were of concern during the lockdown period. As for PM
10, 24 h exceedances occurred at all stations. These exceedances occurred 8 and 33 times at the residential site, 9 and 35 times at the traffic site, and 6 and 29 times at the work site for the GAMEP and USEPA standards, respectively. Similarly, the 24 h exceedances for PM
2.5 occurred at all stations, 56 times at the residential site, 52 times at the traffic site, and 51 times at the work site for the GAMEP and USEPA standards, respectively. Moreover, PM
2.5 and PM
10 had on average more than 75% of the measurements indicated as undesired air quality on the index (
Table 1) and may have affected the health of the inhabitants of Riyadh City.
3.5. Insights for Improving Air Quality
The unintended restriction due to the lockdown could represent an opportunity to better understand potential emission control regulations and strategies and their implications. The concentrations of gaseous criteria air pollutants for the selected weeks were compared to evaluate the extent of these implications.
Figure 6 shows the changes in concentrations of gaseous criteria air pollutants (CO, SO
2, NO
2, and O
3) in residential, traffic, and work sites during the last week of the pre-lockdown period (the week before lockdown was imposed), the first and last weeks of the lockdown period, and the first week after the lockdown. To estimate whether the effects of the lockdown on pollutant concentrations were significant, an unpaired
t-test was used to calculate the pollutant concentrations in the week before the lockdown and the first week of the lockdown (
Table 3). In the traffic site (F-station), the median and mean CO concentrations during the first week of the lockdown period were less than those during the week before the lockdown. The CO mean and median concentrations of the pre-lockdown period decreased by 15% and 36%, respectively, in the first week of the lockdown period at the traffic site. However, this decrease was not significant at the 0.01 confidence level (
Table 3). Moreover, the interquartile range was wider for the first week of the lockdown period than that for the week before the lockdown, reflecting a higher variability in the observed CO concentrations during the lockdown period. This higher variability in CO concentration was due to the low traffic during the lockdown hours and high traffic during hours exempted from the lockdown. The CO concentrations during the first week after the lockdown increased compared with those during the lockdown at the traffic site but did not revert to the levels of the week before imposing the lockdown. This increase was not significant at the 0.01 confidence level (
Table 3).
The CO concentrations during the first week after the lockdown increased compared with those during the lockdown at the work site. This distinct upward change was significant at the 0.01 confidence level (
Table 3). For the residential site (M-station), the CO concentrations exhibited similar trends of weak comparisons as those at the traffic site, except that the CO concentrations during the first week after the lockdown increased considerably compared with those during the lockdown and exceeded the levels of the week before the lockdown. Both the observed decrease in the CO concentrations in the first week of the lockdown period and the increase in the CO concentrations in the first week after the lockdown were significant at the 0.01 confidence level (
Table 3). This suggested that the air quality benefit resulting from controlling CO emissions during this lockdown exhibited significant and more distinct changes in CO concentration levels at the residential and work sites than at the traffic site. Moreover, this change had a longer positive effect on air quality at the work and traffic sites than at the residential site.
NO
2 and SO
2 are directly emitted into the air from fuel combustion and industrial processes. NO
2 concentrations in the traffic site (F-station) decreased by 15% and 18% in the median and mean, respectively, during the first week of the lockdown period and exhibited an interquartile range wider for the first week of the lockdown period than that for the week before the lockdown. The decrease in NO
2 concentrations during the first week of the lockdown period was significant at the 0.01 confidence level (
Table 3). Note that the NO
2 concentrations exhibited a considerable increase during the week before the lockdown ended. During the lockdown period, construction activities were exempted from lockdowns. Consequently, the activities of heavy-duty diesel engines (bulldozers, dump and tanker trucks, compactors, cranes, diesel electrical generators, and road rollers) involved in the construction activities in the city of the Riyadh metro network, which has six lines and 85 stations, increased considerably with extended working hours, attaining a 24 h working mode during the last month of the lockdown period. When the lockdown ended, this considerable increase in construction activities returned to the normal pre-coronavirus operation level. In addition, electricity demand increased; thus, power generation in power plants increased due to progression in warmer conditions as the surface heating increased gradually during the March–May period. Therefore, the NO
2 concentrations during the first week after the lockdown decreased only slightly compared with those during the week before the lockdown at the traffic site. This decrease was not significant at the 0.01 confidence level (
Table 3). For the work site (K-station), the NO
2 concentrations during the first week after the lockdown increased slightly (not significant at the 0.01 confidence level) compared with those during the lockdown. At the residential site (M-station), the NO
2 concentrations decreased significantly during the first week after the lockdown was imposed compared with those during the week before the lockdown and an increase after the lockdown compared with those during the week before the lockdown. The 50th percentile of NO
2 concentrations during the first week of the lockdown period was less than the lower quartile of the NO
2 concentrations during the week before the lockdown. This indicated a significant decrease in the NO
2 concentrations of more than two quarters between the pre-lockdown period and first week of the lockdown period in the residential site. This observed distinct decrease in the NO
2 concentrations in the first week of the lockdown period was significant at the 0.01 confidence level, whereas the increase in the NO
2 concentrations in the first week after the lockdown was not significant at the 0.01 confidence level (
Table 3).
For SO
2, during the first week after the lockdown, the concentration levels decreased only slightly at the residential site (M-station) compared with those during the week before the lockdown. This trend was understandable considering the exemption of construction activities from the lockdown and the gradual increase in power generation during the March–May period. Both the residential site (M-station) and work site (K-station) exhibited significant decreases in SO
2 concentration levels after the lockdown compared with levels observed during the week before the lockdown (
Figure 6 and
Table 3).
For O
3, comparing the last week of the lockdown period with the first week after the lockdown aided in assessing the persistence of the negative effect of the lockdown on elevated O
3 concentration levels.
Figure 6 shows that the O
3 concentrations during the first week after the lockdown decreased only slightly (9.6% and 4.6% decrease in the mean and median, respectively) compared with those during the week before (the last week of the lockdown period).
Overall, the unintended experimental conditions provided by the COVID-19 lockdown provided valuable insights for improving air quality.
Table 3 suggests that applying comparable control measures over one week will result in a decrease of approximately 19% and 15% in the mean CO concentration level at residential and traffic sites, respectively. Similarly, 25% and 18% reduction in the NO
2 mean concentration level can be achieved at residential and traffic sites, respectively. Moreover, the emission control strategies equivalent to the measures implemented during the lockdown over one week could positively affect air quality in terms of controlling CO concentration levels that could last for approximately one week at work and traffic sites and a relatively shorter time at residential sites. Similarly, air quality benefits in terms of a decrease in NO
2 concentration levels over one week could last for approximately one week at work sites and for a relatively shorter time at traffic and residential sites. However, caution should be applied when reducing NO
2 concentration levels because it could result in an increase in O
3 concentrations that could last for over a week in hydrocarbon-limited areas, particularly at work sites (
Figure 6). In addition, strict inspection tests and rigorous standards for the emission compliance and working hours of trucks should be strategized because they can counteract any measures to improve air quality in terms of SO
2 reduction.