Next Article in Journal
Oral Health Barriers for African American Caregivers of Autistic Children
Next Article in Special Issue
A Study of Urban Haze and Its Association with Cold Surge and Sea Breeze for Greater Bangkok
Previous Article in Journal
Analysis of Progressive Muscle Relaxation on Psychophysiological Variables in Basketball Athletes
Previous Article in Special Issue
Artificial Neural Network Modeling on PM10, PM2.5, and NO2 Concentrations between Two Megacities without a Lockdown in Korea, for the COVID-19 Pandemic Period of 2020
 
 
Font Type:
Arial Georgia Verdana
Font Size:
Aa Aa Aa
Line Spacing:
Column Width:
Background:
Article

Spatiotemporal Analysis of Black Carbon Sources: Case of Santiago, Chile, under SARS-CoV-2 Lockdowns

by
Carla Adasme
1,2,
Ana María Villalobos
1 and
Héctor Jorquera
1,2,*
1
Departamento de Ingeniería Química y Bioprocesos, Pontificia Universidad Católica de Chile, Santiago 7820436, Chile
2
Centro de Desarrollo Urbano Sustentable (CEDEUS), Los Navegantes 1963, Providencia, Santiago 7520246, Chile
*
Author to whom correspondence should be addressed.
Int. J. Environ. Res. Public Health 2022, 19(24), 17064; https://doi.org/10.3390/ijerph192417064
Submission received: 15 November 2022 / Revised: 11 December 2022 / Accepted: 13 December 2022 / Published: 19 December 2022
(This article belongs to the Special Issue Advances in Air Pollution Meteorology Research)

Abstract

:
Background: The SARS-CoV-2 pandemic has temporarily decreased black carbon emissions worldwide. The use of multi-wavelength aethalometers provides a quantitative apportionment of black carbon (BC) from fossil fuels (BCff) and wood-burning sources (BCwb). However, this apportionment is aggregated: local and non-local BC sources are lumped together in the aethalometer results. Methods: We propose a spatiotemporal analysis of BC results along with meteorological data, using a fuzzy clustering approach, to resolve local and non-local BC contributions. We apply this methodology to BC measurements taken at an urban site in Santiago, Chile, from March through December 2020, including lockdown periods of different intensities. Results: BCff accounts for 85% of total BC; there was up to an 80% reduction in total BC during the most restrictive lockdowns (April–June); the reduction was 40–50% in periods with less restrictive lockdowns. The new methodology can apportion BCff and BCwb into local and non-local contributions; local traffic (wood burning) sources account for 66% (86%) of BCff (BCwb). Conclusions: The intensive lockdowns brought down ambient BC across the city. The proposed fuzzy clustering methodology can resolve local and non-local contributions to BC in urban zones.

1. Introduction

Black carbon (BC) is one of the components of fine respirable particle matter (PM2.5); it comes from the incomplete combustion of fossil fuels and biomass. Exposure to BC has been linked to short-term [1,2] and long-term [3,4,5,6,7] health effects, but its regulation is indirect through the regulation of ambient PM2.5. Recently, the World Health Organization has updated its air quality guidelines [8], setting an annual average of PM2.5 of 5 μg/m3, which means that long-term BC is implicitly recommended to be well below that guideline since BC is usually below 20% of the total PM2.5.
BC has been traditionally measured offline using thermal-optical methods applied to filter samples [9,10]; these results are reported as total BC in PM2.5 [11]. More recently, continuous instruments based on optical absorption at several wavelengths (from UV to IR) have been developed. These instruments (aethalometers) can apportion BC coming from fossil fuel (BCff) and wood burning (BCwb) combustion because the BC emitted from those sources has a different wavelength dependence for that absorption [12]. This technological development has led to many studies worldwide that report that BC source apportionment in urban [13,14,15,16,17,18,19,20] and rural areas [21,22,23]. Despite this improvement, those apportionment results—on any given receptor site—report the total BCff (or BCwb) coming from local and non-local sources; for instance, regional wildfires may contribute to BCwb as much as local sources, BCff may come from local and regional traffic sources, etc. Additional tools, like air quality models, have been used to resolve those local and non-local BC contributions [24]. Recently, aethalometers have been used to assess the changes in ambient BCff and BCwb associated with urban lockdowns worldwide [25,26,27,28,29,30,31]. All these studies report significant decreases in ambient BC concentrations under those exceptional circumstances, with traffic sources being the largest contributors to those decreases, while BCwb sometimes has not changed [29] or has even increased [32].
The purpose of this work is twofold: (a) report ambient BCff and BCwb concentrations for the very first time in Santiago, Chile, and estimate the reductions in ambient BC concentrations brought by lockdowns during SARS-CoV-2 pandemics, (b) apply a new methodology of spatiotemporal pattern recognition for estimating local and non-local contributions to ambient BCff and BCwb.
The new methodology is based on a fuzzy clustering algorithm applied to ambient BCff and BCwb concentrations along with surface meteorological variables (wind speed and direction, air temperature). This methodology—named FUSTA (Fuzzy SpatioTemporal Apportionment)—splits ambient concentrations into several spatiotemporal patterns, each one corresponding to a contribution from one of the major emission sources [32]. This novel method generates a source apportionment for local and non-local BC sources without the need for air quality modeling applied to the city. The latter would require (a) an accurate emission inventory for BCff and BCwb, (b) the meteorological input fields should be accurate and capture the strong mixing layer seasonality over Santiago, and (c) the air quality model used should not have significant biases.
We find a reduction in total BC in Santiago during the lockdowns in 2020, from 40% to 80%, as compared with previous measurements in 2015; we also find that the FUSTA approach is a useful tool to resolve local and non-local sources of BCff and BCwb.

2. Materials and Methods

The methodology follows a sequential process, as shown in Figure 1. Below, we describe each of the methodological steps.

2.1. Ambient Measurement Campaign

The measurement campaign was carried out between 16 March 2020 and 2 January 2021. Lockdowns started on 27 March in the NE part of the city, and on 23 April, the SW sector of the city was added. Later on 15 May, a total lockdown was enacted until 27 July, followed by less restrictive lockdowns in the city until 30 November, when another rise in people infected forced the government to increase mobility restrictions again [33].
The monitoring was conducted using a multiwavelength aethalometer (MA200, San Francisco, CA, USA) measuring at five wavelengths: 375, 470, 538, 625, and 880 nm, corresponding to ultraviolet, blue, green, red and infrared, respectively. The monitoring site was chosen in a residential area located on the east border of the city (33.406° S, 70.512° W). Surface meteorological data were taken from a nearby site (33.377° S, 70.523° W), which corresponds to an air quality station (Las Condes) run by the Ministry of the Environment [34]. The location of the monitoring site was chosen on the east border of the city to capture the city’s pollution plume arriving at that site when daylight anabatic winds develop. That zone of the city has been studied before with ambient BC campaigns [24], so there was a baseline available to make comparisons with/without lockdowns.
The total BC signal recorded from the instrument was calibrated against the thermal optical transmittance method (TOT) NIOSH 5050 results applied to co-located PM2.5 samples taken on 47 mm quartz filters (Pallflex Tissuquartz 2500QAT-UP, Pall Life Sciences, Portsmouth, UK) using a minivol sampler (Super SASS, MetOne Instruments, Grants Pass, OR, USA); the BC TOT analysis was carried out at Chester LabNet (Tigard, OR, USA).

2.2. Aethalometer Data Analysis

Hourly averages of absorption coefficients (babs) measured at 375 and 880 nm reported by the MA200 are used to compute the Absorption Ångström Exponent (AAE) according to [12]:
AAE = −ln(babs(375 nm)/babs(880 nm))/ln(375/880)
The histogram of hourly values of AAE is analyzed, and the 1st and 99th percentiles are identified with the Ångström exponents for fossil fuel (AAEff) and wood burning (AAEwb), respectively [35]; the estimated values are AAEff = 0.7 and AAEwb = 2.48. Appendix A shows how this estimation was carried out.
Next, the contributions BCff and BCwb are computed as [12]:
BCff = BCtotal·babs,ff(880 nm)/babs(880 nm)
BCwb = BCtotal·babs,wb(880 nm)/babs(880 nm)
where BCtotal is the total BC reading of the instrument at 880 nm, and the following expressions are used to estimate the absorption coefficients babs,ff and babs,wb [12]:
babs,ff(880 nm) = {babs(375 nm) − babs(880 nm)·(375/880)−AAEff}/{(375/880)−AAEwb − (375/880)−AAEff}
babs,wb(880 nm) = {babs(375 nm) − babs(880 nm)·(375/880)−AAEwb}/{(375/880)−AAEff − (375/880)−AAEwb}

2.3. Spatiotemporal Data Analysis

In a previous publication [36], we used bivariate plots and k-means clustering of ambient PM2.5 and PM10, along with receptor model results, to estimate major sources contributing to ambient PM in urban areas; this methodology works best when one or two sources are the major contributors to ambient concentrations. However, this approach has two limitations: (i) the bivariate plots accept only pairs of meteorological variables to analyze ambient PM concentrations, (ii) the clustering technique is hard, that is, each hourly observation may belong to only one cluster (source). To improve the flexibility of that analysis, the meteorological input variables were increased to four: wind speed, wind direction, temperature, and pressure. But the key improvement is to use a fuzzy clustering algorithm, so each hourly observation may belong to more than one (fuzzy) cluster, using the probabilistic concept of cluster membership [37]. The proof of the concept of this new approach (denoted as FUSTA: FUzzy SpatioTemporal Apportionment) was developed for ambient SO2 in an industrial zone, where it was shown that spatiotemporal patterns obtained from FUSTA were like the ones obtained by air quality modeling of the major SO2 emission sources in the study zone [32]. This was the rationale for hypothesizing that FUSTA could resolve local and non-local sources of BCff and BCwb because these are inert tracers of combustion sources, so they are only subject to atmospheric transport and deposition. Below we summarize the major steps needed to carry out such a methodology for the case of black carbon.
Data of BCff and BCwb are log transformed to approach a normal distribution. Each of them is combined with air temperature and pressure and the Cartesian components of wind speed as in the case of bivariate plots [38]. These 5D databases are analyzed to find spatiotemporal patterns in BCff and BCwb by using the algorithm FKM.ent.noise [39] available in the library fclust in the R environment [40]. The following optimization is carried out to find the centroids {C} and membership values U = {uij} for the case of p fuzzy clusters sought:
m i n U , C J F K M N E = i = 1 n k = 1 p u i k · || x i c k || 2 + t · i = 1 n k = 1 p u i k · l o g ( u i k ) + i = 1 n δ 2 ( 1 k = 1 p u i k ) 2 s . t .   u i k [ 0 ,   1 ] ;   k = 1 p + 1 u i k = 1  
where we use the default values t = 1 and δ = 1 in the above equation [39]. The very last term on the right-hand side of (6) stands for a noise cluster, that is, a subset of data that does not follow a regular pattern as the other p fuzzy clusters do [41]. This noise cluster includes outlier values or contributions from intermittent sources like a structural fire or a wildfire plume reaching the monitoring site, for instance.
Once the solution of (6) is found, the BCff estimated at time ‘i’ from Equations (2) and (4) is apportioned as follows:
B C f f i = k = 1 p + 1 B C f f i · u i k = k = 1 p B C f f i ,   k + B C f f i ,   n o i s e    
where B C f f i ,   k stands for the contribution of the k-th cluster (or source) to B C f f i . A similar equation holds for BCwbi. Note that, by design, all those contributions are non-negative.
Since the results are 5D objects, we project the resulting fuzzy clusters using 3 different bivariate plots [38,42,43] in which wind direction is combined with wind speed, temperature, and pressure, respectively, to visualize the spatial distribution of fuzzy clusters found for each BC fraction. These graphs support the task of identifying each of the fuzzy clusters resolved by the FUSTA algorithm (6).
The database and all routines used in the data analysis and visualization are provided as Supplementary Files.

3. Results

3.1. Ambient Monitoring Results

3.1.1. Absorption Ångström Exponents (AAE)

The following table lists the statistics for the estimated absorption Ångström exponents and estimated concentrations of BCff, BCwb and BC for the whole campaign.
Figure 2 shows the diel profiles of AAE for the austral summer and winter months. The winter mean value is significantly higher than the summer value (t = 11.9, p-value < 2.2 × 10−16), which suggests that wood-burning contributions to AAE increase in winter because of residential space heating in the city, a well-known source of ambient PM2.5 in Santiago [44].
Figure 3 shows a comparison of diel profiles of AAE for workdays and weekends. During weekends, the AAE mean value is significantly higher than in the case of workdays (t = 7.64, p-value = 2.8 × 10−14); this suggests a higher consumption of wood burning on weekends and thus the increase in AAE values.

3.1.2. BCff and BCwb Results

Figure 4 shows the time variability for BCff and BCwb contributions estimated from the aethalometer model. BCff is the dominant contribution to total BC all year long; this contribution decreases over weekends, as expected from the traffic activity variability in the city. From Table 1, it follows that, on average, BCff accounts for 85% of total BC. Regarding BCwb contribution (see Figure A3), it rises in winter months, as expected, and it does not decrease over weekends since it comes from residential sources. This contribution does not vanish in the spring and summer seasons; this is explained by wildfires and agricultural burning sources at the regional scale; they have been found in Santiago using receptor modeling of ambient PM2.5 combined with satellite images [45].

3.1.3. Effect of SARS-CoV-2 Lockdowns on BC Concentrations

There is no continuous monitoring of ambient BC in Santiago. However, there was an ambient monitoring campaign that included BC measurements at nearby Las Condes station from December 2014 through July 2015, using an aethalometer (Magee Scientific, Berkeley, CA, USA, model AE33); that campaign results are reported in [24]. Table 2 below makes a comparison of monthly average BC values between that campaign and present results. The most intensive city lockdowns led up to an 80% of reduction in total BC (June 2020), and a 40% reduction has been estimated with fewer intensive lockdowns in December 2020 [33].

3.2. Spatiotemporal Analysis

The fuzzy clustering algorithm of Equation (6) was applied to both datasets of ambient BCx and meteorology (x = ff or wb), and the total number of clusters sought was varied between four and seven clusters—p = 3–6 in Equation (6), respectively. Then, we inspected the time variability of the resulting spatiotemporal patterns (i.e., fuzzy clusters). Based on the similarities in temporal and spatial variability, we identified the major sources contributing to ambient BCx concentrations. Below we discuss the results for both BC components.

3.2.1. Results for BCff

Upon inspection of the different FUSTA results for this BC fraction, the contributions from Santiago’s urban plume arriving at the monitoring site and the noisy cluster contributions were identified by their distinctive upwind locations—W-SW and SSE, respectively (see Figure A4, Figure A5 and Figure 6, below). A residential heating and cooking contribution (RHC) was identified because it is highest overnight when temperatures are lowest—in the winter season. Then, the rest of the contributions are traffic sources located in different directions upwind of the monitoring site. Since the only contribution that vanishes in winter is Santiago’s urban plume, we conclude that all other contributions are local, and they arrive at the monitoring site from different upwind directions and under different combinations of air temperature and pressure (Figure A4, Figure A5 and Figure 6). Table 3 summarizes the mean source contribution estimated in each case. A small variability in major source contribution estimates is observed in these results.
Hence, for simplicity’s sake, we chose the lowest number of fuzzy clusters (5) that apportion all major BCff sources at play. Figure 5 and Figure 6 display the temporal and spatial variability of those clusters, respectively, and Table 4 provides a statistical summary of cluster contributions; additional bivariate plots for BCff are presented in Appendix B (Figure A4 and Figure A5). Below we discuss the features of this five-cluster solution.
Cluster 1 contributions rise in the daylight hours and are zero overnight; these contributions increase in the austral summer season and decrease over weekends. Since they come from W/SW directions, this fuzzy cluster is identified as Santiago’s urban plume reaching the monitoring site as anabatic winds develop during daylight. Contributions of this source are highest when temperatures and wind speed increase in the summer season; this air quality feature of the eastern side of Santiago has been described before [36,46]. On average, this source contributes 14% of the total BCff. Notice that in Table 4, this contribution has more than 25% of hours with zero contribution, which corresponds to overnight conditions.
Cluster 2 contributions increase in the evening hours and reach a maximum before sunrise (when the mixing layer is lowest), are highest in the winter season and low temperatures (Figure A4); they arrive at the monitoring site from different directions (NW–NE) which agree with the highest population density surrounding this site. We identify this source contribution as residential heating and cooking (RHC) sources that use compressed natural gas and liquified petroleum gas as fuels. They contribute on average with 13% of total BCff.
Clusters 3 and 4 rise in the morning, peak in the evening, and decrease until dawn; since they also decrease over weekends, we identify those two clusters as local traffic (TRF) sources. Together they account for 66% of total BCff. These two clusters are resolved by the algorithm because they have different seasonality; cluster 4 contributions are higher when temperatures are lower and winds weaker, so this cluster has the highest seasonality of all.
Cluster 5 includes all sources whose spatiotemporal patterns are intermittent, so they are identified as local combustion sources that peak around 1 pm in winter, most likely associated with residential cooking and heating. On average, this source contributes the least to total BCff, with 7%.

3.2.2. Results for BCwb

We applied the same criteria to identify the contributions of different FUSTA solutions for the BCwb fraction. Thus, we identified Santiago’s urban plume and noise contributions by their distinctive upwind locations—W-SW and SSE, respectively (Figure A6, Figure A7 and Figure 8, below). Once again, only the urban plume contribution vanishes in the winter season—when a low thermal inversion layer blocks air masses from the lower valley from reaching the monitoring site—so the rest of the sources must be local ones. Table 5 shows the mean source contribution estimated for each source as the number of clusters increases. Again, a small variability in major source contribution estimates is observed in these results.
Again, for simplicity, we have chosen to present the results for four (total) clusters in this case. The results are shown below in Figure 7 and Figure 8 and Table 6; additional bivariate plots for BCwb are presented in Appendix B (Figure A6 and Figure A7). Below we discuss the features of this four-cluster solution.
Clusters 1 and 2 have similar diel profiles with peaks in the evening hours but have different seasonality: cluster 1 contributions peak with ambient temperatures lower than 15 °C (Figure A6) and have a stronger seasonality, while cluster 2 contributions have no clear seasonality pattern and are associated to ambient temperatures above 10 °C (Figure A6). We identify these two clusters as local wood-burning sources; the combined contribution is 75% of total BCwb.
Cluster 3 contributions rise in the afternoon and are zero overnight; they peak in the summer season, with high temperatures (Figure A6) and come from W-SW directions. Hence, this is Santiago’s urban plume reaching the monitoring site, and this source contributes 14% of the total BCwb.
Cluster 4 contributions come from S-SE directions and peak in winter around 1 pm, with no weekly seasonality. These contributions come under different synoptic conditions of low and high pressure (Figure A7); they likely come from residential cooking and heating and correspond to 11% of total BCwb. In this regard, this noise cluster has a similar spatiotemporal pattern as the noise cluster found for BCff; this means the residential sources S-SE of the monitoring site contributes to both BC fractions.

3.3. Source Apportionment of BCff and BCwb

The fuzzy clustering methodology (FUSTA) generates a source apportionment of BC at the monitoring site. The following figures show the daily contributions of the different sources resolved in this work; Appendix C presents results for hourly contributions.
Figure 9 and Figure 10 show the daily source contributions for BCff and BCwb, respectively. Local traffic contributions dominate BCff, and local wood-burning sources dominate BCwb. Nonetheless, the noisy source contributions have the largest hourly spikes (Figure A8 and Figure A9). Notice that the urban plume contributions are minimum in wintertime when the mixing layer over the city reaches minimum values [47], blocking air masses from arriving at the monitoring site. The urban plume contribution shows a rise towards the end of 2020, associated with less stringent lockdowns therein and a consequent increase in traffic activity levels [33].

4. Discussion

This is the first report of BC source apportionment conducted in Santiago, Chile that includes the effects of lockdowns brought on by the SARS-CoV-2 pandemics. Hence, the results reported here may be considered a baseline for future studies.
The total BC reductions associated with Santiago 2020 lockdowns—from 40% to 80%—are like the ones estimated for other cities worldwide: Delhi, India [25], up to 78%; Kigali, Rwanda [29], 59%; Sommerville, MA, USA [28], 22–56%; Wuhan, China [31], 39%. One limitation of our estimated reduction is that the baseline is not 2019 but 2015; since ambient PM2.5 has been steadily decreasing in Santiago for the period 2015–2020 [48], this means our estimates are upper bounds (in magnitude) of 2019–2020 BC reductions.
Regarding BC source apportionment during lockdown conditions, BCff is dominant all year long, between 82 and 86% of total BC in Santiago. This is higher than in other cities during lockdowns: 70% in Ahmedabad, India [30], 60–86% in Wuhan, China [31], 51–69% in Delhi, India [25], 50% in Kiwali, Rwanda [29]. We ascribe this to the mild, Mediterranean climate of Santiago, the large fleet of motor vehicles therein and the lower proportion of wood-burning emissions as compared to the above cities.
The non-local contributions coming from the greater Santiago metropolitan area are associated with the development of anabatic winds during daylight hours, so these contributions are zero overnight; the spatial and temporal plots (Figure 5, Figure 6, Figure 7 and Figure 8) show that FUSTA methodology separates this contribution from the local sources. This novel approach circumvents the use of an air quality model to estimate how much BCff (or BCwb) originates locally or is transported from upwind urban sources. In addition, the noisy fuzzy cluster concept handles intermittent sources arriving at the monitoring site, which are local emissions from residential cooking and heating; these are resolved from the other local sources because their spatiotemporal patterns are different. This split of local, non-local and intermittent contributions to ambient BCff and BCwb concentrations will facilitate further air quality modeling studies for these ambient combustion tracer particles.

5. Conclusions

A 2020 baseline of ambient BCff and BCwb concentrations has been compiled for Santiago, Chile, during the SARS-CoV-2 lockdown periods, at an urban site located on the east border of the city. BCff is the dominant contribution all year long, accounting for more than 80% of total BC. During the more restrictive lockdowns, total BC decreased by ~80% compared with a 2015 ambient BC campaign in the same part of the city; likewise, when lockdowns were relaxed, the decrease in total BC reached ~40% on the same comparison basis.
A new methodology to resolve local and non-local BC sources has been developed. This new methodology is based on a fuzzy clustering of ambient observations of BC and four meteorological variables: wind speed and direction, temperature, and pressure. This new methodology (named FUSTA) can resolve different spatiotemporal patterns (i.e., fuzzy clusters) of ambient BC, which arise from different BC sources contributing to ambient BC concentrations at the monitoring site. The methodology resolves, for instance, the arrival of Santiago’s urban plume to the monitoring site due to the daylight anabatic wind regime in Santiago’s basin. Besides, the methodology also handles intermittent sources like residential heating and cooking, especially in the winter season.
The application of FUSTA methodology to ambient BCff and BCwb concentrations has led to the result that local sources are dominant in both BC fractions: traffic and wood burning sources, respectively, with 66% and 75%, respectively. The contributions from Santiago’s urban plume arriving at the monitoring site increased towards the end of the year when lockdowns were relaxed; on average, this contribution reached 14% of BCff and BCwb concentrations. Intermittent residential heating and cooking sources contribute to 7% and 11% of BCff and BCwb concentrations, respectively. When these intermittent contributions are added to the regular spatiotemporal patterns (clusters), the total contribution of local residential heating and cooking sources reaches up to 20% and 86% for BCff and BCwb concentrations, respectively.

Supplementary Materials

The following supporting information can be downloaded at: https://www.mdpi.com/article/10.3390/ijerph192417064/s1, Table S1: Database.csv, a database of ambient BCff, BCwb, and meteorological variables. Macro S1: R_macros.zip, R-software macros to process data and make the fuzzy clustering and post-processing results.

Author Contributions

Conceptualization, H.J.; methodology, H.J. and C.A.; formal analysis, H.J., C.A. and A.M.V.; resources, H.J.; data curation, A.M.V.; writing—original draft preparation, H.J.; writing—review and editing, H.J. and A.M.V.; visualization, C.A. and A.M.V.; All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by ANID, grant number FONDAP 15110020 (CEDEUS), and Grant Fondecyt 1980894.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Data are provided as Supplementary Files (see above).

Acknowledgments

Powered@NLHPC: This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02). We acknowledge the comments and suggestions from three reviewers.

Conflicts of Interest

The authors declare no conflict of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript; or in the decision to publish the results.

Appendix A. Histogram of Absorption Ångström Exponents (AAE) and BC Source Apportionment

Figure A1 shows the histogram of all AAE values estimated using Equation (1) for the whole dataset of ambient measurements. The vertical lines stand for the 1st and 99th percentiles of estimated AAE values.
Figure A1. Histogram of AAE values computed using Equation (1).
Figure A1. Histogram of AAE values computed using Equation (1).
Ijerph 19 17064 g0a1
From this analysis, it follows that the estimated AAE for fossil fuel and wood burning are: AAEff = 0.7 and AAEwb = 2.28, respectively. Using these exponents and applying Equations (2)–(5), the hourly estimates of BCff and BCwb contributions are readily computed for the whole campaign. Figure A2 shows a time plot of those hourly estimates. There is a small number of negative values, which is caused by the extreme values in the above histogram of AAE; when daily averages are computed, no negative BC contributions occur, as shown below in Table A1.
Table A1. Statistical summary of daily average campaign results.
Table A1. Statistical summary of daily average campaign results.
StatisticAAE (-)BCff (ng/m3)BCwb (ng/m3)BC (ng/m3)
Minimum0.8889220112
1st quantile1.07338370470
Median1.14856595668
Mean1.151671123794
3rd quartile1.228807150972
Maximum1.59829385223257
Figure A2. Time plot of hourly BCff and BCwb concentrations, 2020 campaign.
Figure A2. Time plot of hourly BCff and BCwb concentrations, 2020 campaign.
Ijerph 19 17064 g0a2
To help visualize the time variability of BCwb contributions, Figure A3 below shows only BCwb at different time scales.
Figure A3. Time variability of BCwb concentrations, 2020 campaign.
Figure A3. Time variability of BCwb concentrations, 2020 campaign.
Ijerph 19 17064 g0a3

Appendix B. Bivariate Plots for BCff and BCwb Using Temperature and Pressure Instead of Wind Speed

Figure A4. Bivariate plot of hourly BCff contributions, 2020 campaign, using temperature instead of wind speed.
Figure A4. Bivariate plot of hourly BCff contributions, 2020 campaign, using temperature instead of wind speed.
Ijerph 19 17064 g0a4
Figure A5. Bivariate plot of hourly BCff contributions, 2020 campaign, using pressure instead of wind speed.
Figure A5. Bivariate plot of hourly BCff contributions, 2020 campaign, using pressure instead of wind speed.
Ijerph 19 17064 g0a5
Figure A6. Bivariate plot of hourly BCwb contributions, 2020 campaign, using temperature instead of wind speed.
Figure A6. Bivariate plot of hourly BCwb contributions, 2020 campaign, using temperature instead of wind speed.
Ijerph 19 17064 g0a6
Figure A7. Bivariate plot of hourly BCwb contributions, 2020 campaign, using pressure instead of wind speed.
Figure A7. Bivariate plot of hourly BCwb contributions, 2020 campaign, using pressure instead of wind speed.
Ijerph 19 17064 g0a7

Appendix C. Time Series Plots of Hourly Source Contributions to BCff and BCwb

Figure A8. Time series plot of hourly BCff source contributions, 2020 campaign.
Figure A8. Time series plot of hourly BCff source contributions, 2020 campaign.
Ijerph 19 17064 g0a8
Figure A9. Time series plot of hourly BCwf source contributions, 2020 campaign.
Figure A9. Time series plot of hourly BCwf source contributions, 2020 campaign.
Ijerph 19 17064 g0a9

References

  1. Hachem, M.; Loizeau, M.; Saleh, N.; Momas, I.; Bensefa-Colas, L. Short-term association of in-vehicle ultrafine particles and black carbon concentrations with respiratory health in Parisian taxi drivers. Environ. Int. 2021, 147, 106346. [Google Scholar] [CrossRef]
  2. Bista, S.; Fancello, G.; Chaix, B. Acute ambulatory blood pressure response to short-term black carbon exposure: The MobiliSense sensor-based study. Sci. Total Environ. 2022, 846, 157350. [Google Scholar] [CrossRef] [PubMed]
  3. Yang, J.; Sakhvidi, M.J.Z.; de Hoogh, K.; Vienneau, D.; Siemiatyck, J.; Zins, M.; Goldberg, M.; Chen, J.; Lequy, E.; Jacquemin, B. Long-term exposure to black carbon and mortality: A 28-year follow-up of the GAZEL cohort. Environ. Int. 2021, 157, 106805. [Google Scholar] [CrossRef]
  4. Shen, M.; Gu, X.; Li, S.; Yu, Y.; Zou, B.; Chen, X. Exposure to black carbon is associated with symptoms of depression: A retrospective cohort study in college students. Environ. Int. 2021, 157, 106870. [Google Scholar] [CrossRef]
  5. Suglia, S.F.; Gryparis, A.; Schwartz, J.; Wright, R.J. Association between Traffic-Related Black Carbon Exposure and Lung Function among Urban Women. Environ. Health Perspect. 2008, 116, 1333–1337. [Google Scholar] [CrossRef] [PubMed]
  6. Savouré, M.; Lequy, É.; Bousquet, J.; Chen, J.; de Hoogh, K.; Goldberg, M.; Vienneau, D.; Zins, M.; Nadif, R.; Jacquemin, B. Long-term exposures to PM2.5, black carbon and NO2 and prevalence of current rhinitis in French adults: The Constances Cohort. Environ. Int. 2021, 157, 106839. [Google Scholar] [CrossRef] [PubMed]
  7. Ljungman, P.L.S.; Andersson, N.; Stockfelt, L.; Andersson, E.M.; Sommar, J.N.; Eneroth, K.; Gidhagen, L.; Johansson, C.; Lager, A.; Leander, K.; et al. Long-Term Exposure to Particulate Air Pollution, Black Carbon, and Their Source Components in Relation to Ischemic Heart Disease and Stroke. Environ. Health Perspect. 2019, 127, 107012. [Google Scholar] [CrossRef] [Green Version]
  8. World Health Organization. WHO Global Air Quality Guidelines: Particulate Matter (PM2.5 and PM10), Ozone, Nitrogen Dioxide, Sulfur Dioxide and Carbon Monoxide. Available online: https://www.who.int/publications/i/item/9789240034228 (accessed on 10 November 2022).
  9. Cavalli, F.; Viana, M.; Yttri, K.E.; Genberg, J.; Putaud, J.-P. Atmospheric Measurement Techniques Toward a Standardised Ther-mal-Optical Protocol for Measuring Atmospheric Organic and Elemental Carbon: The EUSAAR Protocol. Atmos. Meas. Tech. 2010, 3, 79–89. Available online: www.atmos-meas-tech.net/3/79/2010/ (accessed on 10 November 2022). [CrossRef] [Green Version]
  10. Chow, J.C.; Watson, J.G.; Chen, L.-W.A.; Arnott, W.P.; Moosmüller, H.; Fung, K. Equivalence of Elemental Carbon by Thermal/Optical Reflectance and Transmittance with Different Temperature Protocols. Environ. Sci. Technol. 2004, 38, 4414–4422. [Google Scholar] [CrossRef]
  11. Petzold, A.; Ogren, J.A.; Fiebig, M.; Laj, P.; Li, S.-M.; Baltensperger, U.; Holzer-Popp, T.; Kinne, S.; Pappalardo, G.; Sugimoto, N.; et al. Recommendations for reporting “black carbon” measurements. Atmos. Chem. Phys. 2013, 13, 8365–8379. [Google Scholar] [CrossRef]
  12. Sandradewi, J.; Prévôt, A.S.H.; Szidat, S.; Perron, N.; Alfarra, M.R.; Lanz, V.A.; Weingartner, E.; Baltensperger, U. Using Aerosol Light Absorption Measurements for the Quantitative Determination of Wood Burning and Traffic Emission Contributions to Particulate Matter. Environ. Sci. Technol. 2008, 42, 3316–3323. [Google Scholar] [CrossRef] [PubMed]
  13. Mousavi, A.; Sowlat, M.H.; Hasheminassab, S.; Polidori, A.; Sioutas, C. Spatio-temporal trends and source apportionment of fossil fuel and biomass burning black carbon (BC) in the Los Angeles Basin. Sci. Total. Environ. 2018, 640–641, 1231–1240. [Google Scholar] [CrossRef]
  14. Healy, R.; Sofowote, U.; Su, Y.; Debosz, J.; Noble, M.; Jeong, C.-H.; Wang, J.M.; Hilker, N.; Evans, G.J.; Doerksen, G.; et al. Ambient measurements and source apportionment of fossil fuel and biomass burning black carbon in Ontario. Atmos. Environ. 2017, 161, 34–47. [Google Scholar] [CrossRef]
  15. Küpper, M.; Quass, U.; John, A.C.; Kaminski, H.; Leinert, S.; Breuer, L.; Gladtke, D.; Weber, S.; Kuhlbusch, T.A.J. Contributions of carbonaceous particles from fossil emissions and biomass burning to PM10 in the Ruhr area, Germany. Atmos. Environ. 2018, 189, 174–186. [Google Scholar] [CrossRef]
  16. Liu, Y.; Yan, C.; Zheng, M. Source apportionment of black carbon during winter in Beijing. Sci. Total. Environ. 2018, 618, 531–541. [Google Scholar] [CrossRef] [PubMed]
  17. Helin, A.; Niemi, J.V.; Virkkula, A.; Pirjola, L.; Teinilä, K.; Backman, J.; Aurela, M.; Saarikoski, S.; Rönkkö, T.; Asmi, E.; et al. Characteristics and source apportionment of black carbon in the Helsinki metropolitan area, Finland. Atmos. Environ. 2018, 190, 87–98. [Google Scholar] [CrossRef]
  18. Mousavi, A.; Sowlat, M.H.; Lovett, C.; Rauber, M.; Szidat, S.; Boffi, R.; Borgini, A.; de Marco, C.; Ruprecht, A.A.; Sioutas, C. Source apportionment of black carbon (BC) from fossil fuel and biomass burning in metropolitan Milan, Italy. Atmos. Environ. 2019, 203, 252–261. [Google Scholar] [CrossRef]
  19. Ambade, B.; Sankar, T.K.; Panicker, A.S.; Gautam, A.S.; Gautam, S. Characterization, seasonal variation, source apportionment and health risk assessment of black carbon over an urban region of East India. Urban Clim. 2021, 38, 100896. [Google Scholar] [CrossRef]
  20. Xiao, S.; Yu, X.; Zhu, B.; Kumar, K.R.; Li, M.; Li, L. Characterization and source apportionment of black carbon aerosol in the Nanjing Jiangbei New Area based on two years of measurements from Aethalometer. J. Aerosol Sci. 2020, 139, 105461. [Google Scholar] [CrossRef]
  21. Becerril-Valle, M.; Coz, E.; Prévôt, A.S.H.; Močnik, G.; Pandis, S.N.; Sánchez de la Campa, A.M.; Alastuey, A.; Díaz, E.; Pérez, R.M.; Artíñano, B. Characterization of atmospheric black carbon and co-pollutants in urban and rural areas of Spain. Atmos. Environ. 2017, 169, 36–53. [Google Scholar] [CrossRef]
  22. Stampfer, O.; Austin, E.; Ganuelas, T.; Fiander, T.; Seto, E.; Karr, C.J. Use of low-cost PM monitors and a multi-wavelength aethalometer to characterize PM2.5 in the Yakama Nation reservation. Atmos. Environ. 2020, 224, 117292. [Google Scholar] [CrossRef]
  23. Herich, H.; Hueglin, C.; Buchmann, B. A 2.5 year’s source apportionment study of black carbon from wood burning and fossil fuel combustion at urban and rural sites in Switzerland. Atmos. Meas. Tech. 2011, 4, 1409–1420. [Google Scholar] [CrossRef] [Green Version]
  24. Gramsch, E.; Muñoz, A.; Langner, J.; Morales, L.; Soto, C.; Pérez, P.; Rubio, M.A. Black carbon transport between Santiago de Chile and glaciers in the Andes Mountains. Atmos. Environ. 2020, 232, 117546. [Google Scholar] [CrossRef]
  25. Goel, V.; Hazarika, N.; Kumar, M.; Singh, V.; Thamban, N.M.; Tripathi, S.N. Variations in Black Carbon concentration and sources during COVID-19 lockdown in Delhi. Chemosphere 2021, 270, 129435. [Google Scholar] [CrossRef]
  26. Dave, J.; Meena, R.; Singh, A.; Rastogi, N. Effect of COVID-19 lockdown on the concentration and composition of NR-PM2.5 over Ahmedabad, a big city in western India. Urban Clim. 2021, 37, 100818. [Google Scholar] [CrossRef]
  27. Sonbawne, S.M.; Devara, P.C.S.; Bhoyar, P.D. Multisite characterization of concurrent black carbon and biomass burning around COVID-19 lockdown period. Urban Clim. 2021, 39, 100929. [Google Scholar] [CrossRef]
  28. Hudda, N.; Simon, M.C.; Patton, A.P.; Durant, J.L. Reductions in traffic-related black carbon and ultrafine particle number concentrations in an urban neighborhood during the COVID-19 pandemic. Sci. Total. Environ. 2020, 742, 140931. [Google Scholar] [CrossRef]
  29. Kalisa, E.; Adams, M. Population-scale COVID-19 curfew effects on urban black carbon concentrations and sources in Kigali, Rwanda. Urban Clim. 2022, 46, 101312. [Google Scholar] [CrossRef]
  30. Rajesh, T.A.; Ramachandran, S. Assessment of the coronavirus disease 2019 (COVID-19) pandemic imposed lockdown and unlock effects on black carbon aerosol, its source apportionment, and aerosol radiative forcing over an urban city in India. Atmos. Res. 2021, 267, 105924. [Google Scholar] [CrossRef] [PubMed]
  31. Wang, Q.; Wang, L.; Tao, M.; Chen, N.; Lei, Y.; Sun, Y.; Xin, J.; Li, T.; Zhou, J.; Liu, J.; et al. Exploring the variation of black and brown carbon during COVID-19 lockdown in megacity Wuhan and its surrounding cities, China. Sci. Total Environ. 2021, 791, 148226. [Google Scholar] [CrossRef] [PubMed]
  32. Jorquera, H.; Villalobos, A.M. A new methodology for source apportionment of gaseous industrial emissions. J. Hazard. Mater. 2023, 443, 130335. [Google Scholar] [CrossRef]
  33. ISCI. Urban Mobility Report for Santiago, under SARS-CoV-2 Pandemics. Available online: https://isci.cl/wp-content/uploads/2021/06/Movilidad-RM-Reporte-ISCI-Entel-Ocean-Mayo-2021.pdf (accessed on 27 October 2022).
  34. Ministry of the Environment, Chile. National System of Air Quality Monitoring Information. Available online: http://sinca.mma.gob.cl (accessed on 5 April 2018).
  35. Tobler, A.K.; Skiba, A.; Canonaco, F.; Mockik, G.; Rai, P.; Chen, G.; Bartyzel, J.; Zimnoch, M.; Styszko, K.; Nęcki, J.; et al. Characterization and Source Apportionment of PM 1 Organic Aerosol in Krakow, Poland. Atmos. Chem. Phys. 2021, 21, 14893–14906. [Google Scholar] [CrossRef]
  36. Jorquera, H.; Villalobos, A.M. Combining Cluster Analysis of Air Pollution and Meteorological Data with Receptor Model Results for Ambient PM2.5 and PM10. Int. J. Environ. Res. Public Health 2020, 17, 8455. [Google Scholar] [CrossRef]
  37. Bezdek, J.C.; Ehrlich, R.; Full, W. FCM: The fuzzy c-means clustering algorithm. Comput. Geosci. 1984, 10, 191–203. [Google Scholar] [CrossRef]
  38. Uria-Tellaetxe, I.; Carslaw, D.C. Conditional bivariate probability function for source identification. Environ. Model. Softw. 2014, 59, 1–9. [Google Scholar] [CrossRef] [Green Version]
  39. Ferraro, M.B.; Giordani, P. A toolbox for fuzzy clustering using the R programming language. Fuzzy Sets Syst. 2015, 279, 1–16. [Google Scholar] [CrossRef]
  40. Ferraro, M.B.; Giordani, P.; Serafini, A. fclust: An R Package for Fuzzy Clustering. R J. 2019, 11, 198–210. [Google Scholar] [CrossRef]
  41. Li, R.-P.; Mukaidono, M. Gaussian clustering method based on maximum-fuzzy-entropy interpretation. Fuzzy Sets Syst. 1999, 102, 253–258. [Google Scholar] [CrossRef]
  42. Carslaw, D.C.; Beevers, S.D. Characterising and understanding emission sources using bivariate polar plots and k-means clustering. Environ. Model. Softw. 2013, 40, 325–329. [Google Scholar] [CrossRef]
  43. Grange, S.K.; Lewis, A.C.; Carslaw, D.C. Source apportionment advances using polar plots of bivariate correlation and regression statistics. Atmos. Environ. 2016, 145, 128–134. [Google Scholar] [CrossRef]
  44. Barraza, F.; Lambert, F.; Jorquera, H.; Villalobos, A.M.; Gallardo, L. Temporal evolution of main ambient PM2.5 sources in Santiago, Chile, from 1998 to 2012. Atmos. Chem. Phys. 2017, 17, 10093–10107. [Google Scholar] [CrossRef] [Green Version]
  45. Jorquera, H.; Barraza, F. Source apportionment of ambient PM2.5 in Santiago, Chile: 1999 and 2004 results. Sci. Total Environ. 2012, 435–436, 418–429. [Google Scholar] [CrossRef] [PubMed]
  46. Gramsch, E.; Cereceda-Balic, F.; Oyola, P.; Vonbaer, D. Examination of pollution trends in Santiago de Chile with cluster analysis of PM10 and Ozone data. Atmos. Environ. 2006, 40, 5464–5475. [Google Scholar] [CrossRef]
  47. Muñoz, R.C.; Undurraga, A.A. Daytime Mixed Layer over the Santiago Basin: Description of Two Years of Observations with a Lidar Ceilometer. J. Appl. Meteorol. Climatol. 2010, 49, 1728–1741. [Google Scholar] [CrossRef]
  48. Jorquera, H. Air quality management in Chile: Effectiveness of PM2.5 regulations. Urban Clim. 2021, 35, 100764. [Google Scholar] [CrossRef]
Figure 1. Workflow of the methodology.
Figure 1. Workflow of the methodology.
Ijerph 19 17064 g001
Figure 2. Diel profiles of AAE for (austral) summer and winter months.
Figure 2. Diel profiles of AAE for (austral) summer and winter months.
Ijerph 19 17064 g002
Figure 3. Diel profiles of AAE for workdays and weekends.
Figure 3. Diel profiles of AAE for workdays and weekends.
Ijerph 19 17064 g003
Figure 4. Time variability plot for BCff and BCwb contributions.
Figure 4. Time variability plot for BCff and BCwb contributions.
Ijerph 19 17064 g004
Figure 5. Time variability plot for the five fuzzy clusters’ contributions to BCff.
Figure 5. Time variability plot for the five fuzzy clusters’ contributions to BCff.
Ijerph 19 17064 g005
Figure 6. Bivariate plots for the five fuzzy clusters’ contributions to BCff.
Figure 6. Bivariate plots for the five fuzzy clusters’ contributions to BCff.
Ijerph 19 17064 g006
Figure 7. Time variability plot for the four fuzzy clusters’ contributions to BCwb.
Figure 7. Time variability plot for the four fuzzy clusters’ contributions to BCwb.
Ijerph 19 17064 g007
Figure 8. Bivariate plots for the four fuzzy clusters’ contributions to BCwb.
Figure 8. Bivariate plots for the four fuzzy clusters’ contributions to BCwb.
Ijerph 19 17064 g008
Figure 9. Time plot of daily source contributions to BCff.
Figure 9. Time plot of daily source contributions to BCff.
Ijerph 19 17064 g009
Figure 10. Time plot of daily source contributions to BCwb.
Figure 10. Time plot of daily source contributions to BCwb.
Ijerph 19 17064 g010
Table 1. Statistical summary of campaign results 1.
Table 1. Statistical summary of campaign results 1.
StatisticAAE (-)BCff (ng/m3)BCwb (ng/m3)BC (ng/m3)
Minimum0.0020.620.040.11
1st quantile1.03629455357
Median1.13548890585
Mean1.160690128809
3rd quartile1.237847156988
Maximum3.322781216048679
1 Negative values are excluded from the statistics (see also Appendix A).
Table 2. Comparison of ambient BC measurements in east Santiago, monthly averages (ng/m3).
Table 2. Comparison of ambient BC measurements in east Santiago, monthly averages (ng/m3).
Month2015 12020 3Ratio 2020/2015
January1200
February1063
March1583376 ± 500.24
April2233495 ± 620.22
May2440627 ± 1000.26
June2877533 ± 970.19
July24301207 ± 2790.50
August 1435 ± 196
September 1137 ± 268
October 682 ± 93
November 706 ± 90
December1073 2672 ± 680.63
1 Data adapted from [24]. 2 Data correspond to December 2014. 3 Data reported as mean ± 2σ, estimated from daily averages with at least 75% of valid hourly values.
Table 3. Mean source contributions to BCff (ng/m3) for a different choice of total clusters sought.
Table 3. Mean source contributions to BCff (ng/m3) for a different choice of total clusters sought.
Total ClustersUrban PlumeRHCTRFOther (Noise)
4109unresolved50580
5989045848
6917848640
7875452827
Table 4. Statistical summary of hourly BCff source contributions (ng/m3) for a 5-cluster solution.
Table 4. Statistical summary of hourly BCff source contributions (ng/m3) for a 5-cluster solution.
StatisticCluster 1Cluster 2Cluster 3Cluster 4Cluster 5
Minimum0.00.00.00.00.15
1st quantile0.05.24.50.70.63
Median0.2251.545.024.21.86
Mean98.090.414331547.7
3rd quartile17.4150.82153139.4
Maximum2313641169553046296
Table 5. Mean source contributions to BCwb (ng/m3) for a different choice of total clusters sought.
Table 5. Mean source contributions to BCwb (ng/m3) for a different choice of total clusters sought.
Total ClustersUrban PlumeLocal Wood BurningOther Local (Noise)
4189614
5171038
6151067
7141095
Table 6. Statistical summary of BCwb source contributions (ng/m3).
Table 6. Statistical summary of BCwb source contributions (ng/m3).
StatisticCluster 1Cluster 2Cluster 3Cluster 4
Minimum0.000.00.000.04
1st quantile0.342.370.000.24
Median13.119.10.120.73
Mean64.031.818.414.0
3rd quartile82.649.77.94.1
Maximum8732653871506
Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Share and Cite

MDPI and ACS Style

Adasme, C.; Villalobos, A.M.; Jorquera, H. Spatiotemporal Analysis of Black Carbon Sources: Case of Santiago, Chile, under SARS-CoV-2 Lockdowns. Int. J. Environ. Res. Public Health 2022, 19, 17064. https://doi.org/10.3390/ijerph192417064

AMA Style

Adasme C, Villalobos AM, Jorquera H. Spatiotemporal Analysis of Black Carbon Sources: Case of Santiago, Chile, under SARS-CoV-2 Lockdowns. International Journal of Environmental Research and Public Health. 2022; 19(24):17064. https://doi.org/10.3390/ijerph192417064

Chicago/Turabian Style

Adasme, Carla, Ana María Villalobos, and Héctor Jorquera. 2022. "Spatiotemporal Analysis of Black Carbon Sources: Case of Santiago, Chile, under SARS-CoV-2 Lockdowns" International Journal of Environmental Research and Public Health 19, no. 24: 17064. https://doi.org/10.3390/ijerph192417064

Note that from the first issue of 2016, this journal uses article numbers instead of page numbers. See further details here.

Article Metrics

Back to TopTop