3.1. PCBs
The current study investigated the levels of six indicator PCB congeners (PCB 28, 52, 101, 138, 153, and 180) in yogurt samples collected from 11 Lebanese regions. The results presented in
Table 2 indicate that 40.6% of the tested samples recorded total PCB concentrations exceeding the European Union (EU) maximum residue limit (MRL) of 40 ng/g of fat [
54]. The percentage of individual samples exceeding the MRL within each region ranged from 13.3% (Metn) to 66.7% in Keserwan and 73.3% in South Lebanon, identifying the latter as potential contamination hotspots and demonstrating significant regional variation. Complementing these findings,
Table 3 shows that 59.4% of all samples analyzed had non-detected PCB residues, further emphasizing the variability in contamination levels across regions. Notably, regions such as Metn (86.7%) and Jbeil (80.0%) recorded the highest percentages of non-detected values, indicating relatively lower exposure risk in these areas. In contrast, South Lebanon (26.7%) and Keserwan (33.3%) had the lowest percentages, indicating a higher potential exposure risk.
As presented in
Table 4, the national average of total PCBs was 39.68 ng/g of fat, which is just below the MRL, indicating proximity to the regulatory threshold. However, substantial regional disparities were also observed, reinforcing concerns about the potential health implications for consumers, particularly in high-risk areas.
Among the surveyed regions, Keserwan exhibited the highest mean concentration, reaching 48.15 ng/g fat, followed by South Lebanon (45.91 ng/g fat), North Area (43.56 ng/g fat), Chouf (42.18 ng/g fat), and Baalbek-Hermel (40.58 ng/g fat). These values all surpass the MRL, indicating potential health hazards from prolonged exposure in these areas.
In contrast, other regions such as Metn (32.52 ng/g fat), Batroun (34.19 ng/g fat), Jbeil (35.60 ng/g fat), and Nabatiyeh (37.33 ng/g fat) displayed comparatively lower PCB concentrations, which were all below the regulatory threshold. The variation in total PCB levels is mirrored in the distribution of individual congeners, with PCB153 and PCB180 consistently showing the highest concentrations across most regions, contributing substantially to the total PCB burden.
These quantitative findings are further supported by the box plot presented in
Figure 3, confirming the numerical findings reported earlier and highlighting the regional disparities in the distribution of total PCBs across the studied regions, with several key insights. In the box plot, the circles represent outlying values, which are the observations that lie far from the mid-range of each dataset.
Notably, Keserwan, South Lebanon, North Area, Chouf, and Baalbek-Hermel present with higher medians and broader interquartile ranges, consistent with their mean values exceeding the EU MRL of 40 ng/g of fat. Keserwan shows the widest spread and highest upper whisker, suggesting not only a high median concentration but also a greater variability in contamination within the region. This may indicate heterogeneous exposure sources or varying degrees of environmental persistence and uptake.
South Lebanon and the North Area also display elevated median values and wide ranges, with some values extending above 60 ng/g. Chouf and Baalbek-Hermel similarly show central tendencies above the regulatory limit. In contrast, Metn, Batroun, and Jbeil show lower medians, narrower interquartile ranges, and a more compact distribution, suggesting more uniform and relatively lower contamination levels. Metn, in particular, has the lowest median and contains several outliers, indicating occasional high concentrations in an otherwise low-contamination context. Nabatiyeh also shows modest central values with a notable outlier below 20 ng/g, suggesting localized variation.
According to Cardellicchio et al. [
26], emissions of PCBs into the environment primarily stem from industrial activities, along with improper waste disposal, leakage from landfills, incomplete incineration, and volatilization [
26,
27].
At the local level, Khalil Helou et al. [
17] reported that transformer oils, formerly used by “Electricité du Liban” (EDL), which provide approximately 90% of Lebanon’s electricity, are the primary cause of PCBs pollution in the country. All EDL-managed facilities, including electricity generating sites, distribution stations, and workshops, are recognized as PCB hotspots. These sites encompass a total of 22,551 transformers containing transformer oils distributed across 7 thermal electricity generating stations, 12 hydropower stations, and 58 distribution stations nationwide. According to Shabani [
55], the 7 thermal power plants using oil combustion methods are distributed in the Lebanese territory, as shown in
Table 5.
As shown in
Table 4, the major power plants in Lebanon are located in regions exhibiting the highest levels of PCB contamination in yogurt samples. Among the seven thermal power plants operated by EDL, the Zouk Power Plant, located in Keserwan, is the largest, with an output of 1003 MW. This makes it the most powerful oil-combustion facility in Lebanon.
This is particularly relevant given that Keserwan exhibited the highest total PCB concentration mean (48.15 ng/g fat) among all surveyed regions, well above the EU maximum residue level of 40 ng/g fat. The correlation between the high contamination level and the presence of the largest thermal power plant in the country strongly supports the hypothesis that the Zouk facility is a major contributor to regional PCB emissions.
This association is echoed in other regions as well. For example, South Lebanon, which reported the second-highest PCB level (45.91 ng/g), hosts two power plants: Zahrani (469 MW) and Tyr (70 MW), further confirming the relationship between thermal power generation capacity and environmental PCB load. Similarly, North Area, with a total PCB level of 43.56 ng/g, contains both the Deir Ammar (464 MW) and Hreisheh (75 MW) plants.
The Chouf region, which recorded a total PCB concentration of 42.18 ng/g of fat can be reasonably linked to its proximity to the Jieh power plant, a thermal oil-combustion facility with an output of 622 MW operated by Électricité du Liban (EDL). The Jieh plant is geographically situated along the coast within the administrative boundaries of Mount Lebanon, and in close vicinity to the Chouf district. Baalbek-Hermel also follows this trend, hosting a thermal facility with an output of 70 MW.
These findings reinforce the strong connection between power plant operation, especially facilities using oil combustion with high megawatt output, and elevated PCB concentrations in surrounding areas.
Although the Lebanese Parliament enacted Law 78 in 2018 on the air quality protection [
56], which mandates the establishment of a national ambient air quality monitoring program, emission inventories, and threshold limit values, these provisions have yet to be fully implemented or operationalized in practice. In parallel, approximately 95% of the electricity in Lebanon is generated using fuel-oil in thermal power plants [
57], a practice that significantly contributes to environmental emissions, including greenhouse gases (GHGs) and other harmful pollutants [
58]. This heavy reliance on fuel-oil and gas-oil, coupled with the widespread use of diesel generators and the burning of low-quality fuels for residential and industrial heating, results in the release of persistent organic pollutants (POPs) into the environment. Despite these risks, Lebanon currently lacks binding air quality standards and does not mandate the use of filtration systems for private generators or industrial combustion sources, further exacerbating air pollution and posing serious threats to public health.
In a joint report performed by the UNDP and the Lebanese Ministry of Environment [
59], PCB leakage was reported from improper storage or disposal of electrical equipment or transformer oils, especially in unregulated landfills, which can contaminate nearby soil and water sources affecting local feed and eventually milk supply.
In addition, other environmental sources may also contribute to the regional variability in PCB levels observed in yogurt samples. A study conducted in Tripoli Harbor, northern Lebanon, reported elevated concentrations of 28 PCB congeners across 15 coastal monitoring stations, particularly near port facilities and industrial zones [
60]. These findings suggest that industrial and maritime activities contribute significantly to localized environmental PCB burdens. Such contamination can enter the agricultural chain through multiple pathways, including groundwater used for livestock and irrigation, soil deposition, and atmospheric transport of pollutants, serving as an indirect conduit for PCBs entering the dairy production chain.
On the other hand, the total levels of PCBs remained the lowest in the Batroun and Metn regions, suggesting possibly lower environmental emissions or agricultural contamination in those zones.
Studies investigating PCBs in Lebanon remain very limited, with most focusing on human biomonitoring rather than environmental contamination. For instance, although Harmouche et al. [
20] reported that dairy products were not a significant source of PCB exposure in their urban human biomonitoring study, our findings provide complementary evidence from a food surveillance perspective; by directly measuring PCB levels in dairy fat across multiple regions, we identified significant environmental contamination, particularly in areas near thermal power plants. This suggests that regional environmental factors, rather than consumption habits alone, may drive PCB presence in dairy products, thereby reinforcing the role of local pollution sources previously acknowledged by Harmouche et al. [
20].
Moreover, we have noticed considerable variation in the concentrations of individual PCB congeners across the surveyed regions. For example, PCB28 ranged from 1.679 ng/g of fat in Metn to 3.085 ng/g in Keserwan, while PCB153 ranged from 8.613 ng/g in Batroun to 12.987 ng/g in Keserwan, and PCB180 ranged from 9.900 ng/g in Metn to 14.160 ng/g in Keserwan. Notably, the most frequently detected and abundant congeners across all regions were PCB138, PCB153, and PCB180, which are higher-chlorinated PCBs containing five or more chlorine atoms. These congeners exhibited the highest mean concentrations, measured at 7.502 ng/g for PCB138, 10.024 ng/g for PCB153, and 11.685 ng/g for PCB180 at the national level (
Table 6).
According to
Table 6, the sum of these three high-chlorinated congeners ranged from 25.62 ng/g of fat in Batroun to 35.08 ng/g in Keserwan, while the sum of lower-chlorinated congeners PCB28, PCB52, and PCB101 ranged between 7.92 ng/g in Metn and 13.08 ng/g in Keserwan. On average, the higher-chlorinated PCBs accounted for approximately 74% of the total PCB burden, with PCB180 alone contributing 29.5%, which was the highest proportion among all congeners.
These results are consistent with the congener distribution patterns reported in Harmouche-Karaki et al. [
14], who analyzed PCBs in serum samples of Lebanese adults and found that PCB138, PCB153, and PCB180 accounted for approximately 75% of the total PCBs, with PCB180 alone representing 34.1%. This predominance is in line with the well-documented resistance of these congeners to metabolic degradation. Indeed, PCB138, PCB153, and PCB180 are known to be poorly metabolized compared to lower-chlorinated congeners, which are more susceptible to enzymatic breakdown [
61,
62].
The recurring dominance of these congeners in both dairy and human biological matrices reflect their chemical stability, high lipophilicity, and low metabolic clearance rates. According to the ATSDR, these high-chlorinated PCBs can persist in human adipose tissue for periods ranging from 10 to 47 years, which explains their significant bioaccumulation in lipid-rich compartments such as dairy products, while low-chlorinated PCBs exhibit much shorter biological half-lives, which can reach up to 5 years [
17].
It is important to highlight that, to date, no published data are available on the concentration of PCBs in Lebanese yogurt, and only a limited number of studies have assessed PCB levels in yogurt and other dairy products globally.
Table 7 presents a comparison of non-dioxin-like PCBs (NDL-PCBs) concentrations in milk and yogurt reported in international studies, alongside the findings of the present research. Due to the scarcity of existing studies specifically on yogurt, milk was selected as an additional comparative matrix. This choice is scientifically justified, as yogurt is directly derived from milk, and both share comparable lipid content and contamination pathways, particularly for lipophilic compounds such as PCBs. Therefore, milk serves as a relevant reference matrix to support the evaluation of dietary exposure to PCBs through dairy consumption.
The comparison of our findings with international studies reveals that the mean concentration of PCBs in Lebanese yogurt samples (39.68 ng/g fat) is among the highest levels reported globally, surpassed only by data from Turkey [
67] (127.27 ng/g fat) and significantly exceeding values observed in most European and North American countries. For instance, studies conducted in Canada and Denmark [
10] reported mean concentrations below 2 ng/g fat, while Belgium [
65] and Romania [
66] recorded intermediate levels of 4.72 and 9.12 ng/g fat, respectively. Even in countries with intensive agricultural and industrial activity, such as Spain and Iran [
12,
69], average levels remained substantially lower than those found in Lebanon, with concentrations ranging from 12.55 to 14.65 ng/g fat.
The observed discrepancy highlights a critical gap in environmental and food safety governance. While many countries have implemented effective bans, remediation strategies, and routine surveillance for PCBs, Lebanon continues to face regulatory delays and insufficient enforcement mechanisms. According to Helou et al. [
17], although Lebanon never produced PCBs, widespread historical use of PCB-containing insulating oils in thermal power plants, substations, and transformers operated by EDL has left a lasting legacy of environmental contamination. These infrastructures, distributed across the country, remain major hotspots for PCB release into surrounding ecosystems.
Moreover, the artisanal nature of local dairy production, often lacking formal quality control or standardized feed and water monitoring, may further contribute to contamination through environmental exposure or contact with polluted surfaces. These compounding factors, such as persistent pollution, weak regulatory oversight, and informal food processing practices, likely explain Lebanon’s elevated PCB levels in dairy products when compared to countries with stronger environmental policies and industrial controls.
In light of these concerns, the Ministry of Environment should enhance its oversight of food production activities and promote best environmental practices. Food production facilities, particularly milk processing industries known for their high energy consumption and wastewater generation, must also be pressured to adopt energy-efficient technologies, install proper air filtration systems, and ensure the treatment of wastewater generated during processing. Such measures are crucial for enhancing environmental performance and promoting sustainable practices in food production.
3.2. OCPs
The results of OCP analysis in all yogurt samples collected from the 11 Lebanese regions revealed widespread contamination across all tested OCP compounds, with statistically significant differences observed among regions (
p < 0.001) for most pesticides. The mean concentrations of all OCP compounds in all regions were significantly higher than their corresponding maximum residue limits (MRLs) defined by the Commission Regulation (EU) 299/2008 [
70], suggesting a potential public health concern from dietary exposure to these persistent pollutants. At the regional level, 100% of the samples exceeded the MRL for ΣDDTs, while high exceedance rates were also recorded for α-HCH (95.1%), γ-HCH (89.1%), β-HCH (87.9%), dieldrin (86.7%), methoxychlor (85.5%), HCB (84.9%), and endosulfan (77.6%) (
Table 8). Regional analysis revealed that Bekaa, Baalbek-Hermel, and South Lebanon had the highest frequencies of exceedance for multiple OCPs, pointing to localized sources or agricultural practices contributing to elevated exposure risk. Complementing these findings,
Table 9 shows low non-detection rates for all OCPs, confirming the widespread contamination of yogurt samples. No samples were free of ΣDDTs, and for most compounds, non-detected residues were found in less than 30% of samples. South Lebanon had the highest percentage of samples with non-detected OCPs, with four out of eight compounds showing absence of non-detected results. Similarly, Bekaa and Baalbek-Hermel showed very low non-detection rates across most OCPs. In contrast, Metn recorded the highest non-detection percentages for several compounds, including endosulfan (53.3%), suggesting relatively lower contamination in that region. North Area stood out with a high non-detection rate for endosulfan (96.7%), though detection remained high for other pesticides. These patterns highlight significant regional disparities, likely linked to local agricultural practices.
Specifically, mean concentrations, reported in
Table 10 and
Table 11, across regions were found to be higher than the MRLs of 10 μg/kg for each HCB, α-HCH, β-HCH, and γ-HCH; 50 μg/kg for endosulfan; 10 μg/kg for methoxychlor; and 6 μg/kg for dieldrin. In addition, the levels of organochlorine degradation products, DDT, DDE, and DDD, were markedly elevated across all regions, with total DDT-related compounds (ΣDDTs) far surpassing the MRL of 40 μg/kg fat, further underscoring the contamination burden [
67].
As shown in
Table 10 and
Table 11, regional variation in OCP concentrations is noticed, reflecting differences in agricultural activities and environmental contamination. Regional comparison highlighted that yogurt samples from the Bekaa region exhibited the highest levels of OCPs, followed by Baalbek-Hermel, and the South and North areas. These areas are known for their intensive agricultural practices, which contribute to persistent pesticide residues through soil and water contamination. This aligns with Darwish et al. [
71] who reported that the Central Bekaa Plain, including Baalbek-Hermel governorate, represents Lebanon’s primary region for high-quality farmland. However, intensive agricultural practices, urban development, and industrial activities are putting increasing strain on the area’s already limited soil and water resources [
72].
Moreover, a study performed by El Osmani et al. [
73] has shown that the northern area in Lebanon, which ranks as the second most agriculturally active region in the country, suffers from extensive pesticide misuse given the excessive agricultural activity. The tested groundwater samples were highly contaminated with OCPs, far exceeding Stockholm Convention limits [
73]. The contamination was particularly pronounced during planting seasons, suggesting seasonal spikes due to intensified pesticide use [
73]. This groundwater is commonly used for irrigation and livestock drinking, creating a pathway for OCPs to enter the food chain through contaminated forage and water consumed by dairy cattle.
Similarly, water pollution by OCPs has been documented in other major agricultural zones, including the South Litani River Basin located in the South Lebanon area [
72]. Youssef et al. [
72] reported significant levels of DDE in both surface and groundwater used for agriculture and drinking. These findings underline the persistence of OCPs in the Lebanese water systems and their potential to enter the food chain through contaminated irrigation and livestock drinking water. As dairy cattle consume water and feed from such environments, these contaminants may accumulate in milk fat and eventually appear in yogurt.
These findings align with the national monitoring data presented in the Helou et al. study [
17], stating that agricultural lands constitute primary sites of OCP contamination, such as the Bekaa Plain, North Area, and Akkar.
Lebanon does not manufacture pesticides and entirely ship in all its agricultural needs [
27,
28,
72]. Although the Ministry of Agriculture maintains a registration list for banned pesticides and growth regulators [
74], the country’s agricultural sector faces significant regulatory gaps, including weak market surveillance and inconsistent border control over unauthorized substances. As a result, banned OCPs are still smuggled into the country through official harbors and airports, in addition to uncontrolled segments of the northern and eastern frontiers shared with Syria [
17].
Moreover, OCPs are often misused or mishandled by farmers, who also dispose their containers improperly, which additionally contributes to environmental contamination [
17]. Hence, Lebanon currently lacks the capacity to effectively control both the illegal influx and the improper use of OCPs [
75]. Furthermore, it is evaluated that less than 0.1% of applied pesticides access their target crops, while the majority end up contaminating the air, soil, and water [
75]. Consequently, agricultural fields, along with nearby rivers and streams, are susceptible to being polluted. In Lebanon, gravity-based irrigation is the most common method, which facilitates the transport of OCPs from farmlands into surface and groundwater systems [
17,
75].
Additionally, several studies have documented high pesticide residues in soils across multiple villages, as well as in various vegetable crops such as lettuce, cabbage, tomatoes, and corn, often exceeding their respective MRLs [
44,
76]. This suggests a high likelihood of contamination throughout the broader agricultural environment, including livestock feed. Given that animals often consume locally grown forage and use irrigation water sourced from these areas, contaminated feed represents a critical exposure route. The resulting bioaccumulation in cattle can lead to detectable OCP residues in milk and yogurt, providing a supplementary plausible explanation for the regional contamination patterns observed in our study.
Comparatively, Metn, Batroun, and Jbeil showed relatively lower contamination levels, though still above MRLs, likely due to less agricultural activity and lower pesticide usage in these areas. Nevertheless, even these regions were not exempt from significant contamination, indicating a broader environmental issue affecting the national dairy supply chain.
This widespread environmental contamination explains the presence of OCP residues in the feed and drinking water supplied to dairy cattle. Consequently, these compounds can build up in living beings and increase in concentration up the food web, ultimately contaminating food sources, particularly those of animal origin, and potentially reaching human consumers [
77,
78].
When examining individual compounds across regions, disparities can be observed and are clearly illustrated in
Figure 4 and
Figure 5. As shown in
Figure 3, DDE, DDD, and DDT consistently showed peak levels, particularly in Bekaa (195.33 μg/kg, 155.93 μg/kg, and 124.13 μg/kg fat, respectively) and Akkar (159.76 μg/kg, 150.87 μg/kg, and 126.88 μg/kg fat, respectively). In Lebanon, DDT and its metabolites were banned since 20 May 1998 [
74], and these results suggest both historical persistence and possible ongoing illegal use of DDT and its metabolites despite national bans. Notably the predominance of DDT metabolites followed this order, p,p′-DDE > p,p′-DDD > p,p′-DDT, which is aligned with the half-lives of DDT compounds measured in cows by Fries [
79] who demonstrated that DDE remained persistent, while DDT was converted to DDD through rumen metabolism. This congener pattern is consistent with findings from Helou et al. [
17], who indicated OCP contamination in Lebanese rivers, sediments, and underground water. Particularly, in the Hasbani River, which flows through southeastern Lebanon, DDE was identified as the most prevalent contaminant in three studies, with levels greatly surpassing the maximum permissible limits established by the EPA (8.3 ng/L) moreover its level in the groundwater Hasbani basin exceeded 100 ng/L, which aligns with the peak concentration of DDE found in the yogurt samples collected from the South Lebanon area (189.47 μg/kg fat) [
17]. In addition, the sediment samples from the Kebir river in North Lebanon featured different concentrations of HCB, DDT, and DDE; the highest being DDT with an average sum of 3840 ng/g, aligning with our findings in Akkar (126.88 μg/kg fat), and exhibiting the highest concentration of DDT in the tested samples among other Lebanese regions [
17]. The detection of DDT and its metabolite DDE suggests the long-term environmental persistence of this compound as well as continuous illegal application of this banned pesticide.
Similarly, Endosulfan and β-HCH were widely detected across the surveyed regions, with the highest concentrations observed in the Bekaa, South Lebanon, and Baalbek-Hermel regions (
Figure 5), further highlighting the persistent use of legacy agrochemicals and the lack of effective regulatory oversight. Although Endosulfan was officially banned in Lebanon as of 13 February and 14 December 2010, and β-HCH since 20 May 1998 [
71], their continued presence suggests ongoing illegal use and environmental persistence. Endosulfan concentrations ranged from 53.62 μg/kg of fat in Akkar to 96.73 μg/kg of fat in South Lebanon, with 82% of the regional mean values exceeding the European Union maximum residue level (MRL) of 50 μg/kg of fat. This distribution pattern likely reflects the intensive agricultural practices prevalent in these areas, where Endosulfan may have been historically or illicitly applied for pest control in both crop and animal feed production systems. As for β-HCH, its levels ranged from 53.62 μg/kg of fat in Batroun to 75.75 μg/kg of fat in Bekaa with 100% of mean concentrations exceeding the EU MRL (10 μg/kg fat). α-HCH and γ-HCH followed comparable regional patterns, with the highest values again in Bekaa and Baalbek-Hermel, suggesting either extensive legacy use or environmental persistence. Notably, γ-HCH, also known as Lindane, reached levels as high as 69.99 μg/kg fat in Bekaa, underscoring the widespread distribution of this pesticide.
As presented in
Figure 4, HCB, Methoxychlor, and Dieldrin also exhibited a concerning regional distribution pattern across the analyzed yogurt samples. The highest levels for these compounds were generally concentrated in Bekaa, Baalbek-Hermel, and South and North Lebanon, regions characterized by intensive agriculture. HCB concentrations ranged from 27.75 μg/kg fat in Batroun to a peak of 62.89 μg/kg fat in Bekaa, far exceeding the European Union maximum residue level (MRL) of 10 μg/kg fat. Methoxychlor, although not individually banned in Lebanon, falls under the list of persistent organic pollutants (POPs) prohibited by the Convention of Stockholm, to which Lebanon is a signatory. Its highest concentration was observed in Bekaa (41.49 μg/kg fat). Dieldrin, banned since 20 May 1998, and β-HCH, banned since 24 December 2008 [
74], were also detected at worrying levels. Dieldrin concentrations were particularly elevated in Bekaa (59.95 μg/kg fat), South Lebanon (56.67 μg/kg fat), and Nabatiyeh (51.97 μg/kg fat), far surpassing the MRL of 4 μg/kg fat. These findings highlight not only the lasting presence of these substances in the environment but also the likely continuation of illicit deployment and insufficient implementation of current pesticide policies.
Comparison with biomonitoring data from Helou et al. [
16], which assessed OCP residues in human milk in Lebanon, aligns with the high concentrations of DDE and DDT found in our collected yogurt samples as the most prevalent OCPs in the milk samples were DDT residues (DDT, DDD, and DDE) with DDE detected in 97% of samples. The DDE concentrations in milk ranged from 47 mg/L to 1563 mg/L, and the mean DDE value was 362 ± 34 mg/L [
17].
Similarly, in the Harmouche-Karaki et al. [
14] study, OCPs were evaluated in Lebanese adults’ serum, and DDE was the highest quantifiable compound with a mean concentration value of 18.9 ng/g lipids.
In another study by Harmouche-Karaki et al. [
20], assessing serum OCP levels in Lebanese adults, the findings support the hypothesis that food is the principal transmission route for OCPs. In their study, the consumption of animal-based food, including dairy products, is positively associated with a high level of serum OCP concentrations. This is particularly relevant given that yogurt, a fat-rich food, facilitates the bioaccumulation of lipophilic compounds such as DDT and DDE among other OCPs [
20]. When cattle consume pesticide-contaminated crops, biomagnification occurs along the food chain, resulting in the presence of these chemicals in both meat and milk [
80].
A comparative evaluation of organochlorine pesticide (OCP) residues in yogurt and milk products across several countries, presented in
Table 12 and
Table 13, highlights concerning discrepancies between international and Lebanese levels. In our Lebanese yogurt samples, OCP concentrations expressed on a fat basis were markedly elevated, with the highest concentrations for ΣDDTs, ΣHCH, and Endosulfan reaching 390.22 μg/kg, 179.66 μg/kg, and 70.32 μg/kg fat, respectively. These figures significantly exceed those reported internationally. For instance, in the Middle East, Nida’M et al. [
41] conducted a study in Jordan assessing OCP residues in 233 dairy product samples, including butter, cheese, milk, labneh, and yogurt. Their findings showed that β-HCH, p,p′-DDE, α-HCH, and γ-HCH contaminated 9% (21/233), 8.5% (20/233), 6% (14/233), and 2.1% (5/233) of the samples, respectively [
41]. Heptachlor and α-Endosulfan were present in less than 2% of the tested products [
41]. Aldrin, o,p′-DDD, p,p′-DDD, o,p′-DDE, o,p′-DDT, p,p′-DDT, dieldrin, β-Endosulfan, endrin, and HCB were not detected in any of the samples, contrasting with our findings [
41], where most tested OCP compounds exceeded their respective MRLs in the surveyed yogurt samples. Numerically, Jordanian yogurt and milk samples exhibited values notably lower than those reported in our study: ΣHCH and ΣDDT levels of 94 and 32 μg/kg fat in yogurt, respectively, while milk samples showed levels of 133 μg/kg fat for ΣHCH, 27 μg/kg fat for ΣDDT, and 30 μg/kg fat for Endosulfan [
41]. Whereas research carried out by El Makarem et al. [
42] in Egypt on raw bovine milk samples gathered from three distinct governorates detected the presence of DDT, dieldrin, endrin, and lindane in all samples, with mean concentrations exceeding their respective MRLs; these findings are consistent with the results obtained from our yogurt samples.
In Ethiopia, Ghebremichael et al. [
81] and Deti et al. [
82] reported ΣDDT concentrations ranging between 72.5 and 555 μg/kg fat in cow milk, reflecting significant variability due to geographic and temporal factors. In contrast, European levels were substantially lower. Rodríguez-Hernández et al. [
12] reported ΣHCH, ΣDDT, and Dieldrin concentrations of 0.59, 7.63, and 7.98 μg/kg fat, respectively, in Spanish conventional yogurt, and 0.74, 5.65, and 0 μg/kg fat, respectively, in Spanish organic yogurt, with non-detectable levels of Endosulfan and Methoxychlor underscoring the effectiveness of regulatory controls in the European Union.
When the Lebanese data were presented on a fresh-weight basis to facilitate comparison with the wider literature, the concentrations remained among the highest reported worldwide, reaching 13.66 μg ΣDDT/kg, 6.29 μg ΣHCH/kg, and 2.46 μg endosulfan/kg. Over the past 15 years, Chinese monitoring studies have illustrated the benefits of stringent regulations: the levels of ΣHCH and ΣDDT in milk were 0.60 μg/kg and 0.50 μg/kg, respectively, in 2006 [
83]; they increased slightly to 0.63 μg/kg and 2.29 μg/kg, respectively, in 2017 [
78]; and then they declined to 0.07 μg/kg and 0.10 μg/kg, respectively, in 2021 [
89]. A similar downward trend is evident in India, where concentrations fell from 162 μg ΣHCH/kg, 172.4 μg ΣDDT/kg, and 49.2 μg Endosulfan/kg in 2008 [
84] to ranges of ND–1.24 μg ΣHCH/kg, 0.53–1.70 μg ΣDDT/kg, and ND–1.24 μg Endosulfan/kg in 2020 [
87]. Polish surveys [
85] reported intermediate levels of 1.72–3.75 μg ΣDDT/kg, and 0.72–4.03 μg ΣHCH/kg, while even lower residues were documented in other European countries: Romanian milk [
88] contained only 0.1137–0.218 μg ΣDDT/kg, and Croatian milk [
43] showed 1.04 μg ΣHCH/kg, 1.7 μg ΣDDT/kg, 1.68 μg Endosulfan/kg, 1.78 μg Methoxychlor/kg, and 1.1 μg Dieldrin/kg, underscoring the effectiveness of EU regulatory controls. By contrast, an Egyptian survey [
86] reported markedly higher values of 48.65 μg ΣHCH/kg, 54.77 μg ΣDDT/kg, and 13.96 μg Dieldrin/kg, reflecting continued, largely unregulated use of banned pesticides.
This alarming contrast is further underscored by the environmental context in Lebanon. Although the country does not manufacture OCPs, continued illegal use, smuggling, and inadequate monitoring have led to widespread environmental contamination. This is intensified by artisanal dairy production methods and proximity to agriculturally intensive areas, which likely contribute to higher contamination levels in the dairy supply. These findings, which are in line with Lebanon’s performance on SDG 2, emphasize the urgent need for strengthened regulatory controls, national monitoring programs, and food safety interventions to mitigate exposure risks and align with international standards.
To achieve this, the implementation of a comprehensive “farm to fork” strategy is essential for strengthening traceability, safety, and sustainability across all stages of the dairy value chain, from raw milk production to final consumption. In Lebanon, where food safety oversight is fragmented across institutions [
44], adopting such an integrated approach would improve coordination, reinforce risk assessment, and support compliance with Good Agricultural Practices (GAP), Good Manufacturing Practices (GMP), and Hazard Analysis and Critical Control Points (HACCP) standards. Moreover, it would operationalize the Lebanese Food Safety Law (No. 35/2015) [
45] and help restore public trust in locally produced dairy products.
3.3. Dietary Exposure and Risk Assessment
Table 14 outlines the dietary exposure and possible long-term health risks linked to the consumption of artisanal yogurt in Lebanon, focusing on the analyzed PCB and OCP compounds. To calculate the EDI values, the average concentrations of the compounds were converted to a fresh weight basis using an average fat content of 3.5%, which represents the mean fat content of the yogurt samples analyzed in this study. The fat content across the sampled products ranged between 3.1% and 3.9%, depending on the milk source and production method. While this standardization facilitates comparison with previous studies, it may introduce minor variation in EDI estimations due to natural fat content variability.
The health-based guidance values (HBGVs) used in this assessment include reference doses (RfDs), tolerable daily intakes (TDIs), acceptable daily intakes (ADIs), and provisional tolerable daily intakes (PTDIs), depending on the compound. Specifically, the RfD for ΣPCBs and ΣHCH were set at 20 ng/kg bw/day and 2000 ng/kg bw/day, respectively [
43], and the TDI for hexachlorobenzene (HCB) was 170 ng/kg bw/day as established by WHO/IPCS [
90]. The values for ΣDDTs (10,000 ng/kg bw/day), endosulfan (6000 ng/kg bw/day), and dieldrin (100 ng/kg bw/day) were based on WHO/JMPR ADI and PTDI assessments [
51], while the RfD for methoxychlor (5000 ng/kg bw/day) was derived from U.S. EPA guidance [
91].
The estimated daily intake (EDI) of PCBs from Lebanese yogurt was 1.36 ng/kg body weight/day and is situated within the lower spectrum of EDI estimates reported in Europe according to EFSA [
92], where average exposures range from 4.3 to 25.7 ng/kg bw/day for the sum of six non-dioxin-like PCBs (NDL-PCBs). Comparative data on dietary PCB exposure highlight variations across countries and food sources. A French study from 2012 [
93] observed a low EDI value of 0.046 ng/kg bw/day, with a decline in PCB intake from meat, while dairy products remained a consistent source of exposure. In Austria [
94], estimated PCB intakes ranged from 2.64 to 3.19 ng/kg bw/day for adults, with milk and dairy products accounting for 50–55% of total PCB exposure. Similarly, a study in Turkey [
95] reported lower EDI values of 1.14 ng/kg bw/day for adults and 2.97 ng/kg bw/day for children from milk consumption. In Australia [
96], Total Diet Study results showed EDI ranges of 0.015–2.3 ng/kg bw/day for adults and 0.0032–3.9 ng/kg bw/day for children aged 2–17 years. Compared to these findings, the Lebanese yogurt-based EDI of 1.36 ng/kg bw/day is within the international range, though it is noteworthy given that it stems from a single dairy product. As for the Hazard Quotient (HQ) for PCBs, although the absolute value is relatively low (0.068), it remains a relevant indicator of cumulative exposure, particularly in the context of multiple contaminated food items. Given that dairy products are among the primary contributors to PCB intake, this finding underscores the need for continued monitoring of Lebanese dairy products, especially those from artisanal sources.
For OCPs, EDI values varied between 0.98 and 13.44 ng/kg bw/day, with ΣDDTs exhibiting the highest intake (13.44 ng/kg bw/day), corresponding to 0.13% of the WHO/JMPR HBGV (10,000 ng/kg bw/day) [
51], while methoxychlor is the lowest at 0.98 ng/kg bw/day; intermediate values include ΣHCH (6.16 ng/kg bw/day), endosulfan (2.41 ng/kg bw/day), dieldrin (1.59 ng/kg bw/day), and HCB (1.58 ng/kg bw/day). While all calculated HQs remained well below 1 (ranging from 0.0002 for methoxychlor to 0.0159 for dieldrin), the comparative exposure remains significant. For instance, total diet studies in Croatia [
43] reported EDIs of 3.33 ng/kg bw/day for ΣDDTs, 3.30 for Σendosulfan, 2.04 for ΣHCH, 1.80 for HCB, and 3.49 for methoxychlor. Catalonia milk [
97] exhibited an EDI value of 2.03 ng/kg bw/day HCB; Nanjing adults [
83] received 29.13 ng/kg bw/day ΣDDTs and 12.62 ng/kg bw/day ΣHCH; Hong-Kong milk [
98] contributed 23.8 ng/kg bw/day ΣDDTs and 8.5 ng/kg bw/day endosulfan; and Turkish milk [
95] yielded 2.59 ng/kg bw/day ΣDDTs, 1.86 ng/kg bw/day Σendosulfan, 0.43–1.13 ng/kg bw/day methoxychlor, and only 4.78 ng/kg bw/day ΣHCH.
None of the individual HQs exceeded the threshold value of 1, indicating no immediate carcinogenic health risk from yogurt consumption. However, among the compounds assessed, ΣPCBs (HQ = 0.068) and dieldrin (HQ = 0.0159) demonstrated the highest relative risk indices, suggesting they are the most significant contributors to the overall health risk. Moreover, PCB-153 may also exhibit particular concern, as it was frequently reported as one of the most prominent congeners in various studies, indicating higher environmental persistence and suggesting its disproportionate role in total PCB burden [
99,
100,
101]. Although ΣDDTs had the highest EDI, its HQ remained low due to a high ADI value.
While the present study exhibits non-carcinogenic risk, it is important to highlight that several compounds under investigation, particularly PCB mixtures and dieldrin, are recognized for their carcinogenic potential. According to the International Agency for Research on Cancer (IARC), PCBs are classified as Group 1 carcinogens (carcinogenic to humans) [
102], while dieldrin is classified as Group 2A (probably carcinogenic to humans) [
103]. In addition, the U.S. Environmental Protection Agency (EPA) has established oral cancer slope factors (CSFs) for these substances: 2.0 mg/kg/day
−1 for PCBs [
104] and 1.6 mg/kg/day
−1 for dieldrin [
105]. Although incremental lifetime cancer risk (ILCR) calculations were not conducted in this study, future assessments should incorporate carcinogenic risk on a wide range of food matrices to provide a more comprehensive evaluation of potential long-term public health impacts.
These findings suggest that, even when HQs do not exceed the safety threshold of 1, the consistently elevated EDIs across multiple OCPs in Lebanese yogurt signal a potential cumulative exposure concern. This is especially relevant when considering the lipophilic nature and bioaccumulative behavior of OCPs, which could contribute to chronic health hazards, notably among high-risk populations, including children, expectant women, and high consumers of dairy products. The data underline the urgent need for enhanced surveillance, strengthened enforcement of pesticide restrictions, and broader assessments of dietary exposure from locally produced animal-origin foods.
A key limitation of this risk assessment study is the absence of national consumption data for children and adolescents in Lebanon, which restricted dietary exposure and risk assessments to the adult population. Future research should aim to include younger age groups to better evaluate the risks for more vulnerable consumers.