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This review article examines the levels, sources, and risks of human exposure to polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), and polychlorinated biphenyls (PCBs) in outdoor air across South America. It highlights that urban areas have higher concentrations of these pollutants compared to rural locations, with significant sources identified as biomass combustion, vehicular emissions, and industrial activities. The study calls for improved regulatory measures and continuous monitoring to address the rising levels of these hazardous pollutants.
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0% found this document useful (0 votes)
22 views11 pages

1 s2.0 S0013935125001926 Main

This review article examines the levels, sources, and risks of human exposure to polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), and polychlorinated biphenyls (PCBs) in outdoor air across South America. It highlights that urban areas have higher concentrations of these pollutants compared to rural locations, with significant sources identified as biomass combustion, vehicular emissions, and industrial activities. The study calls for improved regulatory measures and continuous monitoring to address the rising levels of these hazardous pollutants.
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Environmental Research 270 (2025) 120941

Contents lists available at ScienceDirect

Environmental Research
journal homepage: www.elsevier.com/locate/envres

Review article

Current levels, sources, and risks of human exposure to PAHs, PBDEs and
PCBs in South American outdoor air: A critical review
Olumide Emmanuel Akinrinade * , André Henrique Rosa **
Institute of Science and Technology, São Paulo State University (UNESP), Av. Três de Março, 511, Alto da Boa Vista, 18087-180, Sorocaba, SP, Brazil

A R T I C L E I N F O A B S T R A C T

Keywords: This study provides a comprehensive overview of the current levels, sources and human exposure risks to haz­
Persistent organic pollutants ardous polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), and polychlorinated
Stockholm convention biphenyls (PCBs) in South American outdoor air. Research documents were obtainable for only 6 countries
Flame retardants
within the target period (2014–2024). For all contaminants, urban concentrations exceeded that of rural/remote
Organo-halogenated compounds ∑ 3
locations. PAHs were extensively reported with concentration reaching 1100 16PAHs/m in Southwest of
Atmosphere
Buenos Aires province, Argentina. The health risk data also exceeded the threshold level in several locations. The
profiles and seasonal fluctuations across all studies were widely influenced by the prevalent local/domestic
sources. Biomass combustion (particularly of sugar cane/agricultural wastes and wood/coal for residential
heating), vehicular emission, and industrial emission were accounted for most PAH sources. Regulations tar­
geting biomass combustion for improved air quality seem not to currently have significant impacts on current

PAH levels. PBDEs were widely reported within 0.3–55 pg BDE/m3, albeit high concentrations were
∑ 4-14 3
documented in Concepción Bay, Chile (maximum = 1100 pg 4BDE/m ) and Córdoba, Argentina (maximum =

120 pg 4BDE/m3). Most notable source of PBDEs is solid municipal wastes. Similar to other global studies,
BDE-47, 99 and 209 dominated the congeners reported. PCBs were reported with the highest concentrations
∑ 3
measured in Córdoba, Argentina (maximum = 1700 pg 30PCBs/m ), but data remain limited in other
important locations such as São Paulo, Brazil. Sources of PCBs were broadly associated with solid wastes, electric
transformers, and re-volatilization from polluted environment. PAHs, PCBs and PBDEs were all within average to
top global concentrations. This study underscores potential rise in atmospheric level of the target contaminants
without sustainable regulatory structure and the need for continuous monitoring of these contaminants as a
measure of policy impacts. We provide sustainable recommendations.

1. Introduction products particularly electronics and polyurethane foams used in vehi­


cles and furniture (Stubbings and Harrad, 2014; Ma et al., 2024). They
Chemical pollution is a top global priority for addressing public were formulated in three different technical mixtures: PentaBDE
health and environmental concerns. Key among the chemicals are (comprising mainly tetra- and penta-BDE congeners), OctaBDE
polycyclic aromatic hydrocarbons (PAHs) (or polynuclear aromatic (comprising mainly hexa- and hepta-BDE congeners) and DecaBDE
hydrocarbons (PNAs)), polybrominated diphenyl ethers (PBDEs), and (containing BDE-209 as the principal congener and some percentage of
polychlorinated biphenyls (PCBs). PAHs originate from both natural nona- and octa-BDEs), with DecaBDE considered the most widely used
sources, such as forest fires, and human activities. However, anthropo­ PBDEs (Abdallah et al., 2015). Indoor emissions, end-of-life materials
genic sources, majorly from incomplete combustion of carbonaceous and combustion of contaminated products are possible environmental
materials and fuel emissions, are frequently identified as the predomi­ sources of PBDEs (de Souza Araujo et al., 2024; Burgos Melo et al.,
nant environmental contributors (Ma and Harrad, 2015; Jariyasopit 2024).
et al., 2019; Rosa et al., 2024). PCBs were majorly used as dielectric fluids and coolants in electric
PBDEs were historically applied as flame retardants in commercial transformers and capacitors. They also had minor applications in

* Corresponding author.
** Corresponding author.
E-mail addresses: [email protected] (O.E. Akinrinade), [email protected] (A.H. Rosa).

https://doi.org/10.1016/j.envres.2025.120941
Received 29 September 2024; Received in revised form 25 December 2024; Accepted 22 January 2025
Available online 23 January 2025
0013-9351/© 2025 Elsevier Inc. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

lubricating fluids, adhesives, paints, ink products and building sealants


in the indoor environment (Breivik et al., 2002; Zhao et al., 2019;
Akinrinade et al., 2024). Besides deliberate applications, PCBs are also
generated from industrial and thermal processes such as waste inciner­
ation. While most reported cases of PCBs are arochlor-related, there are
increasing reports of non-arochlor PCBs believed to be generated from
sources, such as organic pigments and silicone-rubber production, not
related to the historic PCB applications (Zhao et al., 2019; Anh et al.,
2021; Hombrecher et al., 2021).
Outdoor air serves as a receptor and a medium for long-range, cross-
boundary transport of environmental contaminants. Additionally, pol­
lutants in outdoor air can pose a significant inhalation risk to human
health (Akinrinade et al., 2020). Outdoor air is therefore an important
environmental medium for monitoring of contaminants and impact of
related policies (Wang et al., 2022).
South America accounts for approximately 443 million human
population (Wordometers, 2024). Typical of other global environment, Fig. 1. Number of literature documents reviewed for PAHs, PBDEs and PCBs in
there are several anthropogenic activities and large urban centres in the South American outdoor air.
continent that can generate environmental contaminants such as PAHs,
PBDEs and PCBs considered harmful to human health. Chronic exposure 3. Results
to PAHs has been associated with severe human health challenges
including lung cancer (Aquilina and Harrison, 2023), post-natal depre­ 3.1. PAHs in south American outdoor air
ciation of chest circumference (MoghaddamHosseini et al., 2023) as well
as cardiovascular problems such as thrombosis, atherosclerosis, and 3.1.1. Levels, sources and profiles of PAHs
hypertension (Mallah et al., 2022). Both PCBs and PBDEs are potential The data summarising the concentrations of PAHs in South American
carcinogens and have been listed in the Stockholm Convention on outdoor air are indicated in Tables 1–4 while the levels of the individual
Persistent Organic Pollutants (SC) (Sharkey et al., 2020) while PAHs are PAH compounds are presented in Table S1. Where documented, PAH
regulated under the United Nations Economic Commission for Europe concentrations were generally higher in industrial (Larrea Valdivia
(UN-ECE) on long-range transboundary air pollution (LRTAP) et al., 2019) or urban locations (Arias et al., 2022) relative to rural sites.
(Akinrinade et al., 2020). PAH concentrations were also higher in high-density urban location
The primary objectives of this review are to: (1) understand the compare to less dense urban location (Ceratti et al., 2021). However, no
current level of PAHs, PBDEs and PCBs in South American outdoor air; major difference was recorded for urban and rural concentration in
(2) evaluate the important sources of the contaminants; (3) highlight the Temuco (Chile), highlighting prevailing urban influence of PAH sources
risk implications of these contaminants in outdoor air and proffer rele­ in this location (Pozo et al., 2015).
vant recommendation for future scientific study and sustainable policy PAH sources varied across locations but were widely attributed to
formulation/enhancement. volatilization from contaminated surface, fire outbreaks, biomass com­
bustion (including coal/wood and sugar cane/agricultural wastes);
2. Methods vehicular emission (including that of gasoline/diesel related sources and
gasohol); industrial emission; marine aerosol/ship emissions; as well as
The study documents were obtained from Google Scholar, Scopus military training activities (Tables 1–4).
and Web of Science core collection databases. Literature was initially From Table 1, PAHs in gaseous phase were mostly reported within

searched using the combined keywords: (’’pahs OR pcbs OR pbdes’’ 0.95–52 ng 15-16PAHs/m3. Lighter/mid-light PAHs dominated these
AND ″south america’’ AND ″air OR atmosphere’’). Further searches PAHs, but the specific dominating compounds differed with prevailing
involved replacement of ‘south america’ with the specific names of the PAH sources (Table 1). Where gaseous PAHs were reported simulta­
individual twelve South American countries, that is, Brazil, Colombia neously with particulates, the concentrations in gaseous phase were
(or Columbia), Argentina, Peru, Venezuela, Chile, Ecuador, Bolivia, higher than those in the particulate phase (dos Santos et al., 2020;
Uruguay, Paraguay, Guyana, and Suriname. The study were primarily Galvão et al., 2023; Pereira et al., 2019a) except in Dourados, Brazil,
targeted for 16 USEPA-priority PAHs (Naphthalene (Nap), acenaph­ where lesser gaseous PAHs were reported relative to TSP (Ré et al.,
thylene (Acy), acenaphthene (Ace), fluorene (Flo), phenanthrene (Phe), 2015).
anthracene (Ant), fluoranthene (Flt), pyrene (Pyr), benz[a]anthracene The PM2.5-derived PAHs were reported within the mean concentra­

(BaA), chrysene (Chr), benzo[b]fluoranthene (BbF), benzo[k]fluo­ tion 0.096–18 ng 12-19 PAHs/m3 (Table 2), however, high concen­

ranthene (BkF), benzo[a]pyrene (BaP), benzo[g,h,i]perylene (BghiP), trations were documented in: La Plata, Argentina (mean = 40 ng 14
3
indeno[1,2,3-cd)pyrene (IndP) and dibenz[a,h]anthracene (DBahA)), PAHs/m ) (Mellado et al., 2022); Los Rios Region, Chile (maximum =

however documents reporting >75% of these PAHs were accepted for 120 ng 14 PAHs/m3) (Bravo-Linares et al., 2016a); and Valdivia, Chile

this review. After the initial search, a total of 304 literature were (maximum = 370 ng 14 PAHs/m3) (Bravo-Linares et al., 2016b). The
retrieved between 2014 and 2024. About 75% of the documents were study of Bravo-Linares et al. (2016b) highlighted little/insignificant
found on PAHs and no document was obtained for Paraguay, Venezuela, impact of the policy targeting wood burning restriction on PAH con­
Ecuador, Uruguay, Guyana, and Suriname. After exclusion of the reports centration in outdoor air. PM2.5-bound PAHs were generally dominated
outside the scope of the study, the final documents were limited to forty- with higher molecular weight compounds but the specific compounds
four. Three relevant reports from 2 regional studies (Rauert et al., differ with prevalent sources (Table 2) across the locations. Lighter PAH
2018a;b) as well as 1 global study (Saini et al., 2020) were considered compounds such as Nap and Acy have also been documented (Table 2).
making a total of 47 documents involved in this study. The total number The mean PAH concentrations in PM10 were reported within 2.3–24
∑ 3
of reports finally utilised for each of the target compounds and countries 14-19 PAHs/m while the two reports available for TSP indicated a

is summarised in Fig. 1. concentration range between 2.3 and 39 15-16 PAHs/m3. Nonetheless,
excess concentrations were reported in La Plata (Buenos Aires province),
∑ 3
Argentina (mean = 66 15-16 PAHs/m ) and São Paulo, Brazil

2
O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

Table 1
Concentrations (ng/m3) of gaseous PAHs in South American outdoor air.

Sampling location Sampling period (no of PAHs Concentration of PAHs (ng/ Dominant Major source contributor Reference
samples) m3) mean (range) PAH(s) (s)

Northern-Patagonian oligotrophic 2017 (n = 12) 15 12 (2–39) Phe Pyrogenic Tucca et al.


lake (Concepción Bay) (2020)
Belo Horizonte, Brazil 2017–2018 (n = 100) 16 8.6 Flt, Pyr, & Phe fire outbreak Galvão et al.
(2023)
Belo Horizonte, Brazil 2017–2018 (n = 93) 16 10 Phe, Flu & Pyr Vehicular emission from dos Santos et al.
diesel & gasoline (2020)
Dourados, Brazil 2010 (n = 22) 16 0.95 Nap ns Ré et al. (2015)
São Paulo, Brazil Winter 2016 (n = 30) 15 52 Phe, BaP & ns Pereira et al.
BbF (2019a)
ns
– not specified.

Table 2
Concentrations (ng/m3) of PM2.5 - bound PAHs in South American outdoor air.

Sampling location Sampling period PAHs Concentration of PAHs Major source contributor Dominant PAH(s) Reference
(no of samples) (ng/m3) mean (range)

Southern Metropolitan Area of 2021 (n = ns) 17 17 vehicular combustion IndP & DBahA Narváez-Valderrama et al.
Medellin-Colombia (MAMC) (2024)
Northern Metropolitan Area of 5.3 Nap & Acy
Medellin-Colombia (MAMC)
w
Ribeirão Preto, Brazil 2020–2021 (n = 19) 15 *2.1 (urban) Biomass burning (Phe, BghiP, BbF, Scaramboni et al. (2024)
1.8 (rural) & IndP)
d
(BghiP, BbF,
IndP, Pyr, & Flt)
São Paulo, Brazil Winter 2018 (n = 15 17 (8.8–82) Stationary sources BbF, BkF, & Caumo et al. (2023)
ns) DBahA
Belo Horizonte, Brazil 2017–2018 (n = 16 3.8 vehicular exhaust & Nap, Flu, & BbF Galvão et al. (2023)
100) biomass burning
Rio Grande, Brazil (Industrial) 2009–2010 (n = ns) 16 *0.096 (nd-0.59) – BaP & Pyr Tavella et al. (2022)
Rio Grande, Brazil (Urban) *0.12 (nd − 0.50) –
La Plata (Buenos Aires ns (n = 33) 14 vehicle emissions Ant, BaA, Flu, & Mellado et al. (2022)
province), Argentina 40 Phe
Canoas (Rio Grande do Sul), 2018 (n = 15) 13 3.1 gasoline-powered vehicle Nap Ceratti et al. (2021)
Brazil
Novo Hamburgo (Rio Grande 2018 (n = 17) 0.51
do Sul), Brazil
Belo Horizonte, Brazil 2017–2018 (n = 93) 16 3.8 Biomass, gasoline & Flu & Pyr dos Santos et al. (2020)
diesel burning
rm
Arequipa, Peru 2018 (n = 80) 14 2.1-15 fuel processes & ns Larrea Valdivia et al.
emissions (2019)
São Paulo, Brazil 2014 (n = 32) 19 18 (2.6–62) Exhaust from light duty BbF Pereira et al. (2017b)
vehicles
rm f
Arequipa, Peru 2018 (n = 80) 14 2.1-15 Vehicular emission ns Larrea Valdivia et al.
(2019)
Santo Antônio da Patrulha (Rio 2011–2012 (#n = 9) 16 2.2 (0.66–5.7) Vehicular feet BghiP & IndP da Silva et al. (2015)
Grande do Sul), Brazil
Rio de Janeiro, Brazil 2009 (n = 31) 16 3.8 light-duty vehicles BghiP, BbF, BaP, Oliveira et al. (2014)
fuelled by gasohol & & IndP
diesel
e
Araraquara, Brazil 2010 (n = 16) 12 2.3 (0.61–6.8) Biomass (Sugar cane) BbF, Flu, Pyr, Chr, Souza et al. (2014)
burning & Phe
Los Rios Region (Valdivia), 2013–2014 14 2.8–120 Biomass & vehicular ns Bravo-Linares et al.
Chile emission (2016a)
Valdivia, Chile 2014–2015 (n = 18 3–370 Biomass & vehicular ns Bravo-Linares et al.
140) emission (2016b)
gp
- gas + PM2.5 phase w – wet season d - dry season * - median # - pooled samples.
e
- excluding 53 ng/m3 reported for the nocturnal episode of May 27 ns – not specified rm – range of mean.
f
- 5 & 6 PAH ring.


(maximum = 120 19 PAHs/m3) (Pereira et al., 2017b). These two concentrations were lesser than those observed during the initial
locations were impacted by vehicular emissions (Table 3) with con­ campaign of 2003 and 2008, suggesting a potential long-term reduction
∑ 3
centrations exceeding the 7.2–10 (range of mean) ng 14 PAHs/m in atmospheric PAHs.
documented for the largest open-pit coal mine in Latin America, The PAH concentrations in the combined gaseous and particulate
∑ 3
northern Columbia (Arregocés et al., 2023). phases generally vary within 0.6–110 13-16PAHs/m across South
Increase in PAH levels was observed in São Carlos, Brazil, from 2015 American outdoor air, though excessive concentrations of 28–1100

to 2018 (Carvalho et al., 2023). This observation was related to the (mean = 200) 16PAHs/m3 were registered in Southwest of Buenos
limited impact of legislation aimed at reducing the burning of sugarcane Aires province, Argentina (Orazi et al., 2020). Across the studies, light to
straw and vehicular emissions to curb air concentrations of PAHs. In mid-molecular weight PAHs were frequently reported as dominant PAHs
contrast, comparable PAH concentrations were documented in São (Table 4).
Paulo, Brazil, between 2012 and 2013 (Pereira et al., 2017a), but these

3
O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

Table 3
Concentrations (ng/m3) of PM10 and TSP derived – PAHs in South American outdoor air.

Sampling location Sampling period (no PAHs Concentration of PAHs (ng/ Dominant PAH(s) Major source contributor(s) Reference
of samples) m3) mean (range)

PM10
d
Cuiabá, Brazil 2008–2014 (n = 15 39, w29 BkF & Chr coal/wood/oil combustion & Parra et al. (2024)
149) vehicular emissions
São Carlos, Brazil 2016 (n = 39) 15 1.5 (0.18–7.0) IcdP, BghiP, & BbF, biomass combustion Do Nascimento
et al. (2023)
São Carlos, Brazil 2015–2018 (n = 91) 15 nd - 7.5 BbF & BghiP vehicular emission & biomass Carvalho et al.
rm
(0.98–2.0) combustion (2023)
rm
Largest open-pit coal mine in 2022 (n = 210) 14 7.2 -10 IndP coal/biomass combustion & Arregocés et al.
Latin America, Columbia vehicle emissions (2023)
La Plata (Buenos Aires ns (n = 43) 14 Ant, BaA, Flu, & vehicle emissions Mellado et al.
province), Argentina 40 Phe (2022)
São Paulo, Brazil 2010 (n = 12) 15 23 (6.7–50) BbF vehicular traffic & biomass Pereira et al.
combustion (2019b)
Lima, Peru 2010 (n = 9) 15 2.0 (1.0–3.4) BbF marine aerosol, vehicular,
industrial, & ship exhaust
Medellín, Colombia 2010 (n = 12) 15 8.7 (2.1–15) BbF vehicular, biomass burning, &
industrial sources
rm
Arequipa, Peru 2018 (n = 75) 14 2.3-21 Ant & BghiP wood/coal combustion Larrea Valdivia
et al. (2019)
São Paulo, Brazil 2012 (n = ns) 14 8.2 Phe, DBahA, & Ant vehicular emissions Pereira et al.
Winter 2013 (n = ns) 8.7 BbF & IndP (2017a)
São Paulo, Brazil 2014 (n = 38) 19 24 (5.4–120) BbF exhaust from light-duty Pereira et al.
vehicles (2017b)

TSP

Dourados, Brazil 2010 (n = 22) 16 1.5 Flt, Pyr, BbF, BkF, vehicular emission & biomass Ré et al. (2015)
BaP, & Cry combustion
São Paulo, Brazil Winter 2016 (n = 30) 15 35 BbF, BaP & BkF Vehicular emission & biomass Pereira et al.
combustion (2019a)
rm
- range of mean d-dry w-wet.

Table 4
Concentrations (ng/m3) of PAHs in gaseous and particulate phases reported in South American outdoor air.

Sampling location Sampling period Sampler PAHs Concentration of PAHs Major source contributor Dominant Reference
(no of samples) (ng/m3) mean (range) PAH(s)
rm
Molina, Chile 2014–2016 (n = 6) PAS-PUF 15 28 – 62 (2–110) mixed fossil fuel, biomass & Phe, Flu & Pyr Pozo et al.
combustion (2023a)
g
Belo Horizonte, Brazil 2017–2018 (n = *Active 16 12 vehicular exhaust & fire Flt, Pyr, & Galvão et al.
100) sampler outbreak Phe (2023)
p
Nap, Flu, &
BbF
Yurimaguas, Peru 2019 (n = 12) PAS-PUF 16 6.4 (4.9–9.2) ns ns Esen et al.
(2023)
Concepción Bay, Chile 2013–2014 (n = 8) PAS-PUF 15 0.6–5.5 maritime traffic & military Phe, & Flt Pozo et al.
training activities (2022a)
Tomé (Concepción Bay), 2015 (n = ns) **Active 15 1.3 (0.4–1.7) forest fire & maritime traffic Phe & Flu Pozo et al.
Chile sampler (2022b)
Talcahuano (Concepción 0.9 (0.3–2.2) Ns
Bay), Chile
South West Buenos Aires 2014–2016 (n = 8) PAS-PUF 16 10 (1.1–45) intensive vehicle traffic, Flt, Pyr, BbF, Arias et al.
region, Argentina heating, & other combustion & BkF (2022)
activities
Southwest of Buenos Aires 2015 (n = ns) PAS-XAD-2 16 200 (28–1100) pyrolytic sources Nap & Phe Orazi et al.
province, Argentina (2020)
rm
Yurimaguas, Peru 2018 (n = 12) PAS-PUF 16 14-31 coal & biomass combustions ns Sari et al.
(2020a)
Santiago de Cali, 2011 (n = ns) PAS-PUF 13 25–66 vehicular traffic & forest fires Phe, Flt, Pyr Álvarez et al.
Colombia (2016)
#
Dourados, Brazil 2010 (n = 22) Active 16 2.1 (0.38–8.5) vehicular emission & biomass Nap, Pyr, & Ré et al.
sampler combustion Phe (2015)
Temuco, Chile 2008–2009 (n = 6) PAS-PUF 15 nd-70 residential wood combustion, Phe, Flt & Pyr Pozo et al.
industrial & vehicular emissions (2015)
rm
- range of mean ns – not specified g – gaseous phase *gas + PM2.5 ** gas + not specified particulate #
gas + TSP.

3.1.2. Seasonal concentrations of PAHs coal heating and lower boundary layer heights preventing dispersion of
For all the air phases, concentrations of PAHs across different seasons pollutants (Bravo-Linares et al., 2016a; Bravo-Linares et al., 2016a;
was mainly influenced by the dominant anthropogenic activities for Tucca et al., 2020). Similarly, high PAH concentrations were reported in
each season. Maximum concentrations were mostly documented in dry season (Carvalho et al., 2023; Scaramboni et al., 2024) or summer
colder season/period in climate regions as a result of residential wood/ (Galvão et al., 2023) in tropical regions with annual or frequent fire

4
O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

outbreaks in addition to less atmospheric wet deposition. However, in­ The dominant PAH associated with health risk vary with sources
fluence of high vehicular traffic has been reported to increase PAH across sampling locations. However, BaP, DBahA, BaA, and IndP were
concentration in wet season (dos Santos et al., 2020) and in other re­ frequently identified as the major risk contributor (Table S6).
ports, significant difference was not observed for PM2.5-derived PAHs
across the season (da Silva et al., 2015; dos Santos et al., 2020). 3.1.5. Comparison of health risk implications of PAHs in south American
outdoor air and those of other global locations
3.1.3. Diagnostic signatures and other source appropriation tools utilised The health risk data obtained for selected global locations are sum­
for PAHs in south American outdoor air marised in Table S7. The BaPeq in Table S7 is generally within
Patterns of PAH-related environmental activities, source diagnostic 0.03–0.75 ng/m3, which is consistent with the widely reported values
ratios (Tables S2 and S3), and multivariate statistical tools such as for South American air (0.039–0.82 ng/m3) (Table S6). However,
principal component analysis (PCA) exploiting various PAH source excessive concentrations were reported in Dhaka, Bangladesh (19–150
markers (Table S4) were commonly utilised for PAH source identifica­ ng/m3), Yangon & Mandalay, Myanmar (mean = 12 ng/m3) (Zhang
tion. These can be supplemented by backward air mass trajectories of et al., 2024); and Gdynia city, Poland (maximum = 9.6 ng/m3) (Siudek,
the NOAA (National Oceanic and Atmospheric Administration)’s HYS­ 2023). These high concentrations are below the reports in São Paulo
PLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) pro­ (Brazil) (mean = 23 ng/m3) (Pereira et al., 2019a) and Cuiabá (Brazil)
gramme and wind rose plot, to identify remote or distance sources. (mean = 19 ng/m3) but PAHs in Dhaka (Bangladesh) significantly
PCA however has limitations for source quantitation making statis­ exceed all the PAHs reported for South America. Similar dominant PAH
tical tools/programmes such as positive matrix factorisation (PMF) compounds were accounted for the BaPeq (BaP, DBahA, BbF, BaA &
(positive matrix factorisation (PMF)) and polytopic vector analysis IndP) except Flt additionally identified in Molina (Chile) and BghiP
(PVA) (Bravo-Linares et al., 2016b) additional tools for receptor models. identified in Rio Grande do Sul (Brazil).
However, both PMF and PVA require sufficient large number of samples Similar to the BaPeq, the ILCR reported in Table S7 is within
relative to the number of target compounds (Scaramboni et al., 2024). acceptable risk (<10− 4) for most studies accessed, except in Dhaka
Although commonly utilised for source appropriations, several lim­ (Bangladesh) (mean = 9.4 × 10− 3) and Yangon & Mandalay (Myanmar)
itations have been reported for both diagnostic ratio and PAH source (0.4–1.3 × 10− 3). Besides, these two locations, the ILCR reported in São
markers. PAHs are posed to photodegradation and are subject to Paulo, Brazil (Caumo et al., 2023; Pereira et al., 2017a, 2019b); Cuiabá,
chemical reactions/oxidation with atmospheric species such as ozone, Brazil (Parra et al., 2024); Canoas (Rio Grande do Sul), Brazil (Ceratti
OH radicals, and nitrogen oxides in low troposphere (dos Santos et al., et al., 2021); and Medellín, Colombia (Pereira et al., 2019b; Mueller
2020). These factors are likely to significantly influence the level of PAH et al., 2019) exceed those of other reports in Table S7.
species identified for broad class or specific source/sources. For Data available in Tables S6 and S7 suggest that the health risk im­
example, Ant photodegrades faster than Phe subjecting Ant/(Ant + Phe) plications of PAHs in South American outdoor air is within the average
to a less conservative ratio under long-atmospheric transportation. to top category of other global reports.
Similarly, BghiP photodegrades faster than IndP; BaP and BkF are also
prone to photoreaction in the presence of visible light (Orazi et al., 2020; 3.2. PBDEs in south American outdoor air
Do Nascimento et al., 2023). Other influencing factors are phase changes
driven mainly by temperature, and peculiarity of fuel compositions, The air concentrations of PBDEs reported on South America as well
particularly mixed fuel such as gasohol (Pereira et al., 2017b; Oliveira as the dominated congener(s) are summarised in Table S8; the maximum
et al., 2014). Despite these limitations, PAH diagnostic ratio and source concentrations reported for each location are indicated in Fig. 2 while
markers remain widely used and important tools for PAH source the individual compounds of the 8 most commonly reported congeners
appropriation. are presented in Table S9.

3.1.4. Health risk associated with PAHs in south America outdoor air 3.2.1. Concentrations and sources of PBDEs in south American outdoor air
The present study focused on the broad toxicity assessment of the PBDEs in South American outdoor air were widely reported between
∑ 3
atmospheric-related PAHs mainly through inhalation route, other 0.3 and 55 pg 4-14BDE/m . Albeit, excessive concentrations were

toxicity evaluations involving mutagenic estimation and dermal or documented in Concepción Bay, Chile (maximum = 1100 pg 4BDE/
ingestion route were infrequent and were not considered in this study. 3
m ) (Pozo et al., 2022a) as well as Córdoba, Argentina (maximum = 120
∑ ∑
The full descriptions of the algorithms and models involved in the health pg 4BDE/m3) Córdoba, Argentina (maximum = 120 pg 4BDE/m3)
risk assessment of the atmospheric PAHs are provided in supplementary (Pegoraro & Wannaz, 2019). The high concentration reported in Con­
information (Equations (1)–(4)). The two key parameters involved for cepción Bay was primarily attributed to debris resulting from the 2010
these risk assessments were BaPeq (Benzo(a)pyrene-equivalent) and Tsunami event.
Incremental lifetime lung cancer risk (ILCR). Values of BaPeq exceeding In a comparative global study, GAPS (Global Atmospheric Passive

1 ng/m3 or ILCR exceeding 10− 5 is considered to have significant cancer Sampling) network reported 12–18 pg 3
9BDE/m for the South
risk implication (Alani et al., 2021). American countries with São Paulo (Brazil) registering the highest
The health risk data of the atmospheric PAHs in South America as concentration while the minimum concentration was recorded in Bogota
well as the principal PAH contributors are summarised in Table S6. No (Colombia) (Saini et al., 2020). These concentrations are consistent with
specific trend in terms of the air phase can be identified in the health risk the previous reports in the GRULAC region where nd – 20 pg
∑ 3
implications as risks are mostly related to the studied environment, 14BDE/m was documented for the South American countries (Rauert
procedure for health risk evaluation, sampling techniques and target et al., 2018a). High concentrations were observed in Chacaltaya, Bolivia

PAHs. Both BaPeq and ILCR were widely reported within acceptable/ (maximum = 20 pg 14BDE/m3), Concepción, Chile (maximum = 18 pg
∑ 3 ∑ 3
low risk values (Table S6). However, excessive risks were documented in 14BDE/m ), and São Luis, Brazil (maximum = 15 pg 14BDE/m )
several locations including Sao Paulo, Brazil (Pereira et al., 2017a, (Fig. 2) (Rauert et al., 2018a).
2017b, 2019a, 2019b; Caumo et al., 2023), Canoas (Rio Grande do Sul), Ship-based air measurements have also been reported within the port
Brazil (Ceratti et al., 2021), Cuiabá, Brazil (Parra et al., 2024), Medellín, of Mar (del Plata city, Argentina) and over the South Atlantic Ocean off
Colombia (Pereira et al., 2019b) and Molina, Chile (Pozo et al., 2023a). the coast of South America with concentrations ranging between 0.7 and

Although BaPeq was not evaluated, high BaP values were reported in La 2.6 (mean = 1.8) pg 10BDE/m3 (Pegoraro et al., 2016). PBDE con­
Plata (Buenos Aires province) and Argentina (Giuliani et al., 2021) centrations declined from the continental shelf over the shore demon­
(Table S2). strating the influence of continental/regional air mass on atmospheric

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O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

Fig. 2. Maximum concentrations of PBDEs in South American outdoor air


c = number of congeners
La pintana = La Pintana, Ñuñoa, Cerrillos & San Bernardo
∑ 3 ∑ 3
Excessive concentrations reported at Concepción Bay, Chile (maximum = 1100 pg 4BDE/m ) and Córdoba, Argentina (maximum = 120 pg 4BDE/m )
are excluded.

PBDE concentrations. significantly exceed similar report around Santa Marta landfill in Chile
PBDE concentrations were infrequently evaluated for exposure risks. (child = 0.01–0.01; adult = 0.04–0.33 pg/(kg-bw.day) (Pozo et al.,
Only one information was obtained around Santa Marta landfill, Chile 2023b) (Tables S8 and S10). Other data summarising the concentrations
(Pozo et al., 2023b) with estimated inhalation daily exposure doses of PBDEs in selected global outdoor air are shown in Table S10 while
(DEDs) of 0.01–0.33 pg/(kg.day). These levels were significantly below Table S11 indicates the congener profiles of the 8 commonly reported
USEPA reference doses of 7000, 200, 100 and 100 ng/(kg.day) for PBDEs.

BDE-209, BDE-153, BDE-99, and BDE-47 congeners, respectively; as The concentration of 12–18 pg 9PBDE/m3 reported in four South
well as 3000 and 2000 ng/(kg.day) for the octa-BDE and penta-BDE American cities (São Paulo - Brazil, Bogota - Colombia, Santiago - Chile
homologues, respectively (United States Environmental Protection and Buenos Aires - Argentina) alongside other global mega-cities, is

Agency USEPA, 2014). consistent with that of Kolkata (India) (17 pg 9PBDE/m3) but below

Sources of PBDEs were typically linked to debris (Pozo et al., 2022a) those of Madrid (Spain) (22 pg 9PBDE/m3), Toronto (Canada) (39
∑ ∑
and open combustion of contaminated municipal solid waste pg 9PBDE/m3), New York (USA) (110 pg 9PBDE/m3), London (UK)
∑ ∑
(Miglioranza et al., 2021; Pozo et al., 2023b). There is a notable limited (88 pg 9PBDE/m ), and Mexico city (35 pg 9PBDE/m3) (Saini et al.,
3

information regarding seasonal concentrations of PBDEs; however, the 2020). Similarly, a study in the GRULAC region (Rauert et al., 2018a),
data available in Rauert et al. (2018b) indicate no significant changes in indicated high concentration in Mexico (maximum = 130 pg/m3)
the seasonal concentrations of PBDEs in South American outdoor air. compared to other South American countries (Columbia - 14 pg/m3,
Brazil - 15 pg/m3, and Argentina - 18 pg/m3) but low concentration was
3.2.2. Profiles of PBDEs in south American outdoor air reported for Costa Rica (0.34 pg/m3).

BDE-209 was commonly reported as the principal PBDE congener PBDE concentrations in Córdoba, Argentina (34–120 pg 9PBDE/
3
(Tables S8 and S9). This is related to the high global applications and m ) (Pegoraro & Wannaz, 2019) were below similar reports on Bir­

late restriction of DecaBDE (only included in the SC in 2019) with the mingham (UK) (range of mean = 100–490 pg 8PBDE/m3) (Drage et al.,
exception for use in some applications. Another plausible factor is the 2016), but the maximum concentration elevates another study in Bir­
involvement of particulates in the studies as BDE-209 is known to mingham taken during the Covid-19 event (maximum = 59

partition mostly to particles (Pozo et al., 2017). pg 7PBDE/m3) (Rosa et al., 2024).
Other commonly reported dominant congeners are BDEs – 47 and 99 The PBDE concentrations in Lagos (Nigeria), 21–750 (median = 100)

(Tables S8 and S9) which are key components of PentaBDE commercial pg 8PBDE/m3 (Akinrinade et al., 2022), New Delhi (India) (mean =

formulations. BDE-47 is also likely to dominate in long-distance/rural 200 pg 8PBDE/m3) (Chakraborty et al., 2017), and Harbin (China)

locations over BDE-209 due to higher volatility of BDE-47 and strong (2–320 pg 13PBDE/m3) (Qi et al., 2014) exceed all other reports on
partitioning of BDE-209 to particles which are likely to deposit closer to South America except Concepción Bay (Chile), where excessive 1100

the respective sources (Pozo et al., 2017). pg 4PBDE/m3) was reported (Pozo et al., 2022a).

3.2.3. Comparison of the PBDE levels in south American outdoor air and
those of other global locations 3.3. PCBs in south American outdoor air
This comparison was initially targeted at exposure/inhalation risk,
however due to limited available risk data, comparison was mainly The available data for PCBs in South American outdoor as well as the
based on concentrations as proxies for risk assessment. However, where major reported homologues are summarised in Table S12; the maximum
reported the exposure risks via inhalation route (child = 1.54; adult = levels reported in each location are indicated in Fig. 3; while the data
0.61 ng/(kg-bw.day)) in Gauteng, South Africa (Katima et al., 2018) capturing individual seven indicator congeners are presented in
Table S13.

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O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

Fig. 3. Maximum concentrations of PCBs in South American outdoor air


c = number of congeners.

3.3.1. Concentrations and sources of PCBs in south American outdoor air et al. (2016) indicated that PCB concentrations did not decline over a
The PCB congeners targeted in most studies vary significantly with 10-year period, likely due to the buffering of PCBs from polluted sur­
∑ 3
reported concentrations ranging within 0.4 7PCBs/m - 1700 pg faces. Similarly, the GRULAC reports (Rauert et al., 2018a) showed no
∑ 3
30PCBs/m (Table S12). High concentrations were typically found in significant difference between 2014 and 2015. However, a decline in
industrial or urban locations compared to remote, downtown, rural or regional concentrations was observed when compared to earlier GRU­
agricultural sites (Tombesi et al., 2014; Álvarez et al., 2016; Astoviza LAC reports.
et al., 2016; Pozo et al., 2017; Silva-Barni et al., 2018; Pegoraro &
Wannaz, 2019; Miglioranza et al., 2021). Urban areas are often associ­ 3.3.2. Profile of PCBs in south American outdoor air
ated with fresh PCB signatures originating from sources such as electric PCB profiles differ across locations (Tables S12 and S13) reflecting
equipment or combustion. In contrast, the PCB concentration in sub­ the sources and congener pattern of the specific arochlor mixture used
urban/rural areas relates to long-range transportation and re-emission (Sari et al., 2020b). Low molecular weight homologues/congeners (di-to
from sink sources such as contaminated soils (Astoviza et al., 2016; tetra-CBs) were widely attributed to long-distance sources or secondary
Pozo et al., 2017). emission/re-volatilization from contaminant surfaces (Silva-Barni et al.,
PCB sources were widely attributed to: old electrical equipment/ 2018) while higher molecular weight PCBs, mostly above tetra-CBs,
transformers containing PCB fluids such as Arochlor 1254 (Álvarez were commonly associated with close sources due to high potential for
et al., 2016; Silva-Barni et al., 2018; Pegoraro & Wannaz, 2019) particulate portioning and short distance transportation of particulates
including those present in hydroelectric dams (Miglioranza et al., 2021); (Tombesi et al., 2014; Astoviza et al., 2016; Pegoraro et al., 2016; Pozo
volatilization from contaminated surface (Astoviza et al., 2016; et al., 2017). Generally, tri to tetra-CBs, particularly PCB-28 and 52, are
Miglioranza et al., 2021; Esen et al., 2023) including lake (Luarte et al., the commonly reported homologues.
2022); and open combustion of solid municipal wastes (Silva-Barni
et al., 2018; Ruggeri et al., 2020).
While long term study is largely missing, the reports of Pegoraro

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O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

3.3.3. Comparison of the concentration of PCBs in south American outdoor and harmonisation of these risk models for accuracy and comparison
air and those of other global locations purposes.
Table S14 summarises the data of PCBs in outdoor air of the selected 3. For adequate measurement of policy impacts and risk assessment of
global locations while the individual congeners of the seven indicator air contaminants, we recommend consistent study of PAHs, PCBs and
congeners are shown in Table S15. PBDEs in outdoor air across the South American continent and other

Regionally, the maximum 52PCB concentration in (Celestún) global locations. Such study should focus on full seasonal period and
Mexico (maximum = 130 pg/m3) and Sonora (Mexico) (maximum = accommodate gas plus particulate phases to avoid underestimation
110 pg/m3) exceed that of all other South American countries reported of level and risk assessment.
(Tables S13 and S14) (Rauert et al., 2018b). However, extremely low 4. For all contaminants, we recommend future research to accommo­

concentration was reported in Tapanti (Costa Rica) ( 52PCB 0.08–0.34 date specific congeners for easy comparison and monitoring for
3
pg/m ). temporal and long-term trend.
The concentration of the seven indicator PCBs in Chile (3.4–19 pg/ 5. The available studies on South American continent focused exten­
m3) (Pozo et al., 2022b) is consistent with the background concentration sively on PCB congeners found in historic commercial technical-

in Waldhof (mean = 6.9 pg 6PCB/m3) and Schmücke (mean = 8.4 mixture (arochlor-PCBs). However, there are increasing reports of
∑ 3
pg 6PCB/m ), Germany (Dreyer and Minkos, 2023). Similarly, PCB non-arochlor PCB congeners with sources unrelated to the conven­
concentrations (0.4–36 pg/m3) in Santiago, Concepciόn, & Temuco in tional commercial-mixture. We recommend that future studies in
Chile (Pozo et al., 2017) and North-Patagonian lakes of Chile (3.1–43 South America should focus on these congeners and their sources.
pg/m3) (Luarte et al., 2022) are within those of King George Island, West 6. Different acronyms were used across literature particularly for the
Antarctica (0.91–36 pg/m3) (Wang et al., 2017). However, all the in­ 16 USEPA PAHs. We recommend harmonising these acronyms for
dicator PCBs reported on South America are significantly lower than simplicity and to avoid misrepresentation.
similar reports in Nigeria (23–280 pg/m3) (Akinrinade et al., 2022) and
remote location of the Canadian Great Lakes Basin (18–110 pg/m3) 5. Conclusion
(Shunthirasingham et al., 2016).
Considering other congeners, the maximum concentration reported Extensive PAH contaminations were reported across Columbia,

for Santiago de Cali (Colombia) (850 pg 18PCB/m3), Southern Río de la Argentina, Peru, Brazil and Chile, with health risk exceeding threshold

Plata Basin (Argentina) (940 pg 42PCB/m3) (Astoviza et al., 2016), and level in several locations. Comparatively, health risk data are within

Córdoba (Argentina) (1700 pg 30PCB/m3) (Pegoraro & Wannaz, 2019) average to top category of other global locations. Prevalent PAH sources

are substantially higher than that of 510 pg 40PCB/m3 in Bursa, were identified as biomass combustion (particularly of sugar cane/
Turkey. However, Cetin et al. (2017) reported excessive PCB concen­ agricultural wastes and coal/wood for residential heating in cold sea­

tration of 4200 pg 41PCB/m3 which elevated all concentrations re­ son), vehicular, and industrial emissions. Seasonal fluctuations of PAHs
ported in South America as well as other PCB data obtained in this study. were largely influenced by prevalent sources for the specific season or
Although different congeners were targeted across the studies location. Relevant regulations targeting wood/coal/agricultural waste
limiting adequate comparison, the available evidence suggest that PCB combustion currently have limited impacts on air PAH concentration.
concentration in the South American outdoor air did not differ from the PCB and PBDE concentrations are generally reported within average
average to the top level of other global concentrations. The homologue to top global concentrations. Literature however remain insufficient for
profiles of PCBs in South American outdoor air also did not significantly both PCBs and PBDEs in several important locations such as São Paulo,
differ from those of other locations (Tables S12–S15). However, di-PCB Brazil. PBDE sources were mostly assigned to municipal solid wastes.
and other homologues related to non-arochlor sources are likely to have Meanwhile PCB sources were associated with waste combustion,
substantial relevance in atmospheric concentration and transportation. contaminated electrical transformers as well as re-volatilization from
This is due to unintentional input of the related congeners from sources secondary sources. Dominant BDEs- 47, 99 and 209 were frequently
such as organic pigment and silicone-rubber production site (Zhao et al., reported signifying the relevance of Penta- and DecaBDE commercial
2019; Anh et al., 2021; Hombrecher et al., 2021). Although different formulations in the atmospheric concentrations of PBDEs in South
non-arochlor PCB congeners have been reported particularly PCB 11, America. Although tri to tetra-CBs homologues, particularly PCB-28 and
47, 51, 68, and 209, high proportion have been frequently observed for 52, commonly dominated the PCBs reported, PCB profiles are largely
PCB-11 (Zhao et al., 2019; Anh et al., 2021). No report was found on related to source contributors and distance transportations.
non-archlor PCBs in South American outdoor air in this study. No report was found for Paraguay, Venezuela, Ecuador, Uruguay,
Guyana, and Suriname.
4. Priorities for future research
CRediT authorship contribution statement
The following are recommended for future research and policy
formulation/enhancement: Olumide Emmanuel Akinrinade: Writing – review & editing,
Writing – original draft, Visualization, Methodology, Investigation,
1. PAH source markers and molecular diagnostic ratios remain key Formal analysis, Data curation, Conceptualization. André Henrique
tools for the identification of PAH sources. However, these tools can Rosa: Writing – review & editing, Visualization, Supervision, Method­
be less conservative as a result of: (a) factors that are likely to in­ ology, Investigation, Funding acquisition, Conceptualization.
fluence PAH in the outdoor environment such as gas-particle parti­
tioning (driven by temperature) and atmospheric reaction/ Declaration of competing interest
oxidation/photodegradation; (b) different sources within similar
categories captured by the source marker/diagnostic ratio; and The authors declare that they have no known competing financial
unique sources such as blended fuels. Studies highlighting appro­ interests or personal relationships that could have appeared to influence
priate use and identification of relevant source markers/diagnostic the work reported in this paper.
ratios are required for all possible scenarios.
2. PAH health risk models are important mechanisms for examining Acknowledgments
health implications of atmospheric PAHs. Current assessment
methods are too diverse suggesting some level of inadequacy and The authors thank the National Council for Scientific and Techno­
difficult comparison across literature. We recommend robust study logical Development (CNPq), Coordination for the Improvement of

8
O.E. Akinrinade and A.H. Rosa Environmental Research 270 (2025) 120941

Higher Education Personnel (CAPES) and Sao Paulo Research Founda­ of atmospheric particulate matter in the city of São Carlos, Brazil. Chemosphere 326,
138450. https://doi.org/10.1016/j.chemosphere.2023.138450.
tion (FAPESP, grant numbers 2023/15847-0; 2023/14685-7; 2023/
Caumo, S., Yera, A.B., Alves, C., Casotti Rienda, I., Kováts, N., Hubai, K., Vasconcellos, P.
09923-6) for financial support and granting the fellowship of O.E. C., 2023. Assessing the chemical composition, potential toxicity and cancer risk of
Akinrinade. airborne fine particulate matter (PM2.5) near a petrochemical industrial area.
Environ. Toxicol. Pharmacol. 101, 104170. https://doi.org/10.1016/j.
etap.2023.104170.
Appendix A. Supplementary data Ceratti, A.M., da Costa, G.M., Alves, D.D., Cansi, L.M., Hansen, J., Brochier, F., de
Quevedo, D.M., Osorio, D.M.M.O., 2021. Polycyclic aromatic hydrocarbons (PAH) in
Supplementary data to this article can be found online at https://doi. atmospheric particles (PM2.5 and PM2.5–10): integrated evaluation of the
environmental scenario in urban areas. Water, Air, Soil Pollut. 232, 30. https://doi.
org/10.1016/j.envres.2025.120941. org/10.1007/s11270-020-04967-3.
Cetin, B., Yurdakul, S., Keles, M., Celik, I., Ozturk, F., Dogan, C., 2017. Atmospheric
Data availability concentrations, distributions and air-soil exchange tendencies of PAHs and PCBs in a
heavily industrialized area in Kocaeli, Turkey. Chemosphere 183, 69–79. https://
doi.org/10.1016/j.chemosphere.2017.05.103.
No data was used for the research described in the article. Chakraborty, P., Zhang, G., Cheng, H., Balasubramanian, P., Li, J., Jones, K.C., 2017.
Passive air sampling of polybrominated diphenyl ethers in New Delhi, Kolkata,
Mumbai and Chennai: levels, homologous profiling and source apportionment.
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