For all measured pollutants, the overall correlation coefficient between the PLFs and the reference instruments was often weak (r<0.4). Moderate correlation coefficient with the reference instruments was observed with one of PLFs at indoor location (r = 0.58) and two of PLF at roadside location (0.4 < r < 0.6) when measuring PM2.5, but not for PM10 and NO2 concentrations. When analyzing only a subset of the data when the high pollution periods were observed during the Guy Fawkes Night (POPS measurement showed a maximum of 118.7 μg/m3), 11 PLF units showed stronger regression results (R2 values > 0.5) with a one-hour compared to a one-minute (n=9) for PM2.5 . For the full indoor measurement period (3 weeks), 4 PLF units showed stronger regression results (R2 values > 0.5) for PM2.5. PM10 and NO2 showed consistently poor regression results (R2 values < 0.5) in both the raw (1 min), 1 hour averaged, for both the high pollution period and for the full measurement interval.
3.1. Indoor Monitoring
Figure 1 shows measured time series of PM
2.5, PM
10, and NO
2 by the reference instrumentation, POPS and ARISense (first column) and 3 PLF devices (PLF2, PLF11, and PLF12) out of 17, illustrating their highly variable performance. The series for the remaining 14 PLF devices are shown in
Figure S1.
The reference indoor air quality instruments show strong variability in concentrations over the full measurement period. Levels of air pollution exceeded the WHO threshold during periods from October 20 to November 16, 2020 with a high exceedance detected by the POPS device at 9:24 PM for PM
2.5 pollutant with a level of 118.77 μg/m
3 (
see Figure 1A). The PM
10 and NO
2 reference monitor readings also revealed a significant peak that exceeded the WHO threshold of 242.5 μg/m
3 and 59.13 ppb, respectively. This occurred during Guy Fawkes Night from November 5, 2020 at 5:00 PM to November 6, 2020 at 3:00 AM (highlighted with a blue line), and the event also had a clear effect on the indoor air quality at this time. Outdoor air quality has a significant impact on indoor air quality, especially evident when indoor sources of pollution are absent [
24]. Natural ventilation, open windows and doors, are the most prevalent ways for outside air to enter and influence indoor environments.
Figure 1A, the high and low PM
2.5 readings of the PLFs (PLF11 and PLF12) generally coincided with the PM
2.5 concentrations measured by POPS. However, they did not follow the reference ARISense for PM
10 and NO
2 concentrations, as shown in
Figure 1B,C. PLF2, for instance, showed inconsistent tracking patterns (high-frequency readings that exceed the WHO threshold) in comparison to the references for PM
2.5, PM
10, and NO
2 levels. Most of the other PLFs, as shown in
Figure S1, exhibit the same unreliable multiple high peak patterns during this time.
The summary statistics of the indoor monitoring pollutants measured by the PLFs and the POPS and ARISense instruments are shown in
Table S1. The mean of indoor PM
2.5 concentration reading taken by POPS over the duration of indoor sampling (three weeks) was 6.21 μg/m
3, while that of PLFs ranged between 3.39 and 8.06 μg/m
3. On the other hand, PM
10 mean concentration from ARISense was 16.7 μg/m
3, and that of PLFs ranged between 8.39 and 34.85 μg/m
3. The mean of indoor NO
2 reading concentration taken by ARISense was 6.91 ppb, while that of the PLFs ranged between 13.1 and 21.08 ppb.
Overall, the correlation coefficient average between the PLFs and the references was very weak (r values less than 0.4), indicating poor agreement (Supplemental digital content:
Tables S4–S6). There was a moderate correlation between PLF and POPS reference for only one PLF unit (PLF19) (r = 0.58), the remining 16 of the 17 PLF revealed a weak degree of agreement for the PM
2.5 (see
Table S4). PM
10 and NO
2 concentration data measured by the PLFs revealed no to very weak agreement (0.005 < r < 0.29) and (0.02 < r < 0.22), respectively.
Table 1,Figure 2,
Figure 3 and Figure 4 show the results of the regression analyses for each PLF. The range of the PLFs’ R
2 values for PM
2.5 is 0.0–0.63, PM
10 is 0.0–0.05, and for NO
2, it is 0.00–0.05. The RMSE value range is 3.2–8.8 for PM
2.5, 20.2–47.5 for PM
10, and 13.1–28.7 for NO
2. For the PM
2.5 measurements, 13 out of 17 PLFs have lower R
2 values (below 0.5; close to 0) and higher RMSE values (far from zero), this suggests that the regression model has a relatively weaker goodness of fit and less accurate prediction, indicating a poor measurement performance of the PLF sensors. Exceptional have been seen in 4 PLF units (PLF11,12,13, and 19), for which R
2 values ranged between 0.45 and 0.63 (R
2 close to 1), and their RMSE values range between 3.4 and 4.2 (RMSE close to 0), indicating that all of the variance in the four PLF units is explained moderate to substantial portion of the variance in the references and the model’s predictions have relatively small deviations from the actual observed values, which suggesting a better measurement performance for PM
2.5. The performance of all PLFs, not limited to those four units, showed poor measurements for PM
10 and NO
2.
Specifically looking at the performance of PLF11 and PLF12, in
Figure 1, where PLF11 and PLF12 seem to show reasonable performance with the PM
2.5 variations as recorded by POPS, the error value metrics (R
2 and RMSE) also improved. Their R
2 and RMSE values are 0.58 and 3.4 and 0.58 and 3.6, respectively. The PM
10 and NO
2 variation from those two personal units still performed poorly (see
Figure 1B,
C). The poor linear responses were observed for all PLFs regarding PM
10 and NO
2, including those two units (PLF11 and PLF12, see
Figure 3 and Figure 4). Their R
2 and RMSE values are (0.05 and 20.2), and (0.03 and 26.1), respectively, for PM
10, and (0.00 and 22.7), and (0.05 and 14.0), respectively, for NO
2.
Figure 4.
Regression plots for PLFs and ARISense reference device for the 1-min NO2 concentrations carried out over a month at the indoor monitoring location. X-axis represents ARISense reference instrument; Y-axis represent PLFs tools; ----: Blue line represents the linear regression fit line between the measured NO2 concentrations from PLFs and ARISense; ----: Black line represents the 1:1 line. The equation for the linear regression is (Y = bX + a); R2 = coefficient of determination.
Figure 4.
Regression plots for PLFs and ARISense reference device for the 1-min NO2 concentrations carried out over a month at the indoor monitoring location. X-axis represents ARISense reference instrument; Y-axis represent PLFs tools; ----: Blue line represents the linear regression fit line between the measured NO2 concentrations from PLFs and ARISense; ----: Black line represents the 1:1 line. The equation for the linear regression is (Y = bX + a); R2 = coefficient of determination.
Table 2 show regression results comparing 1-min and 1-hour over the full indoor measurement period (3 weeks). During this period only 4 out of 17 PLFs showed better performance results (R
2 values > 0.5, highlighted with gray in
Table 2) when measuring PM
2.5 levels with a 1-minute, and 1 out of 17 PLFs performed better (highlighted with blue in
Table 2) with a 1-hour. R
2 values for PM
10 and NO
2 showed poor performance (R
2 values < 0.5) in both 1 min and 1 hour.
Similar have been seen for the short-time period (5 days) that included high levels of pollution (the Guy Fawkes Night event), see
Table 3. During this period of high pollution 9 out of 17 PLFs showed better performance results (R
2 values > 0.5, highlighted with gray in
Table 3) when measuring PM
2.5 levels with a 1-minute, and 11 out of 17 PLFs performed better (highlighted with blue in
Table 3) with a 1-hour. R
2 values for PM
10 and NO
2 showed poor performance (R
2 values < 0.5) in both 1 min and 1 hour.
It is clear that, 1-hour intervals and during the selected high pollution period, 11 (out of 17) of the PLFs demonstrate some measurement proficiency. For example, the PM
2.5 R
2 values for PLF12 are 0.58 (1-min measurements for three weeks period in
Table 2), 0.68 (1-min measurements for five days in
Table 3), 0.75 (1-hr for five days). An earlier study that tested the same type of tools showed similar results[
22]. In their study, they found that only three and four devices (out of 32) gave high precision (80 – 100%) for PM
2.5 and PM
10, respectively.
3.2. Roasdside and supersite intercomparison
PM
2.5 pollution levels were measured only at the roadside with the POPS instrument, and PM
2.5, PM
10 and NO
2 levels were measured at the Supersite. Due to the short time period of the measurements, only descriptive and correlation coefficient analyses for each site were conducted. At the time of measurements, the air quality measurements at both sites (road and Supersite locations) showed concentrations lower than the WHO 24-hour mean limit value (see
Figures S2 and S3). An elevated concentration of PM
2.5 was observed for periods between 3:30 PM and 3:41 PM (November 13, 2020), as detected by POPS at the roadside location for PM
2.5, with the maximum level reaching 18.60 μg/m
3 (
see Figure 4A).
Figure 4.
Time series of POPS and Supersite monitors (reference) and three PLF tools for PM2.5, 1-min concentrations carried out for over three hours at the (a) roadside and (b) Manchester Air Quality Supersite. ---- : Red dash line represents the WHO limited value (15 µg/m3 for 24-hr mean PM2.5).
Figure 4.
Time series of POPS and Supersite monitors (reference) and three PLF tools for PM2.5, 1-min concentrations carried out for over three hours at the (a) roadside and (b) Manchester Air Quality Supersite. ---- : Red dash line represents the WHO limited value (15 µg/m3 for 24-hr mean PM2.5).
Tables S2 and S3 provide a summary of the roadside and Supersite pollutants measured by the PLFs, and references POPS and Supersite instruments. The roadside mean concentration of PM
2.5 recorded by PLFs ranged between 2.4 and 18.54 μg/m
3 (maximum of 12.54–75.18 μg/m
3), while the mean concentration of 7.12 μg/m
3 (maximum of 18.6 μg/m
3) with measurements taken by POPS. Findings from the Supersite location, the mean concentration of PM
2.5, PM
10, and NO
2 recorded by PLFs ranged between 2.12 and 7.72 μg/m
3 (maximum of 11.25–78.91 μg/m
3), 8.14 and 27.59 μg/m
3 (maximum of 115.41–572.93 μg/m
3), 1.8 and 23.89 ppb (maximum of 15.97–183.3 ppb), respectively, while the mean concentration was 3.05 μg/m
3, 6.48 μg/m
3, and 9.92 ppb (maximum of 4.13 μg/m
3, 8.8 μg/m
3, and 18.38 ppb) for PM
2.5, PM
10, and NO
2, respectively with measurements taken by the Supersite monitors.
Despite the short measurement periods in the outdoor environments, the measured pollutant levels obtained from the PLFs (n= 15 units) do not show a good correlation (r < 0.4) with the concentrations measured by the POPS and supersite instruments at both locations. Exceptional results were seen with two PLFs (PLF2 and PLF17) that showed moderate correlation (0.4 < r < 0.6) when measuring PM
2.5 at roadside location. The correlation tables for the road and Supersite locations are given in the supplementary material (see
Tables S8 and S9).
Our field evaluation results show, at best, a weak correlation between the majority of the PLF devices (n=16) and the reference instruments for all measured pollutants. Only one PLFs showed a moderate correlation with the reference data. Our results are in agreement with another field evaluation reported by the South Coast AQMD [
23]. Their R
2 for PM
2.5 measurement between 0.02 and 0.15 for three PLF units and a Federal Equivalent Monitor GRIMM (FEM GRIMM) over an hour period, and was stronger over 24 h of observation (0.02 < R
2 < 0.72) compere to 5 min (0.01 < R
2 < 0.09) [
22].