Impact of Various Smoking Techniques on Polycyclic Aromatic Hydrocarbon (PAH) Formation in Dry-Cured Pork Neck (Buđola)

Abstract

Traditional meat products that are smoked may pose health risks due to polycyclic aromatic hydrocarbons (PAHs). Recently, concerns have grown about the health implications of meat products smoked under traditional, uncontrolled conditions. This study compares the levels of polycyclic aromatic hydrocarbons in specimens of the dry-cured meat product “Buđola” made in traditional smokehouses versus industrial chambers. PAHs were measured upon completion of smoking and when the production was complete. The findings indicate that traditional smoking methods lead to higher PAH contamination compared to industrial methods. Among the 16 PAHs analyzed, 10 (NA, AL, FL, ANT, PHE, FLT, BA, PR, BBF, BKF) were detected in traditionally smoked “Buđola” samples, whereas only 2 (NA, AL) were found in samples smoked by industrial methods. The BP levels in all samples were undetectable. PAH4 levels in industrial smoked “Buđola” were below the quantification limit, while those in traditional products were 28.77 μg·kg⁻¹ for the surface layers and 21.14 μg·kg⁻¹ for inner layers. The total PAH16 content ranged from 4.32 μg·kg⁻¹ to 3587.83 μg·kg⁻¹. The inner layers had lower concentrations of overall and specific PAHs in relation to the product surface. The results suggest that, from a health perspective, industrially produced “Buđola” is safer for consumption than the product smoked in uncontrolled conditions.

1. Introduction

Smoking meat is one of the oldest methods of meat preservation, and in Herzegovina, this method of preserving is very widespread and prolongs the shelf life, while creating characteristic flavours and aromas in products [1,2,3]. Traditional delicacies made from smoked meat are of great importance in the economy of the meat industry; up to 60% of meat products are submitted to some form of smoking [1]. All these processes can, however, create polycyclic aromatic hydrocarbons (PAHs) at the same time, a class of chemical compounds well known for their carcinogenic properties, casting a shadow on the safety of smoked meats [4]. PAHs result from the incomplete combustion of organic material such as wood used in smoking and can accumulate in meat. Especially in traditional methods of smoking, where open fireplaces and natural wood prevail, the concentrations of PAHs are higher than in industrial techniques of smoking [2,4]. These methods enhance the taste and texture in some meats, like Buđola, but at the same time, present significant health risks due to the build-up of PAH compounds such as benzo[a]pyrene (BP), which is related to the increased incidence of cancer [5]. Consequently, controlling smoking conditions to reduce PAH levels is critical for consumer safety [6].

The study of PAH formation in smoked meats has recently taken on a new importance, in particular, after the issuance by the European Commission of regulations establishing upper limits for PAHs in smoked meat products. A maximum limit of less than 2 μg·kg⁻¹ was established for benzo[a]pyrene (BP) and up to 12 μg·kg⁻¹ for the combined amount of PAH4: benzo[a]anthracene (BA), chrysene (CHY), benzo[b]fluoranthene (BBF), and benzo[a]pyrene (BP) [7]. From 2020, EU member states allow higher limits compared to those stated above for traditional products, values up to 5 μg·kg⁻¹ in the case of BP and up to 30 μg·kg⁻¹ regarding PAH4; however, concerns remain high, above all in traditionally smoked meats like “Buđola” [8]. The study of the levels of PAHs in smoked meats presents a wide variety of factors that each affect the formation of these compounds, including the type of wood being used, length and temperature of smoking, fat content, placement of products in the chamber, and casing. These studies show that by regulating each of these parameters, the PAH content in smoked meats can be significantly reduced [9,10,11,12]. Other traditionally smoked meats, such as sausages and hams, were reported in previous studies to contain PAHs. Results showed risks of traditional smoking as opposed to industrial techniques with liquid smoke or more controlled environments [13,14,15,16]. On the other hand, “Buđola” is a traditional smoked meat product originating from Herzegovina that is widely consumed and has a certain risk in its production process about which little attention has been given so far. This present study tries to fill this knowledge gap by conducting tests on the effects of different smoking techniques on PAH formation in “Buđola”. Comparisons of traditional versus industrial smoking will be performed by measurements of PAH concentrations, and furthermore, an assessment of health risk. The obtained results are expected to give an indication of how the smoking procedure can be optimized based on the minimal formation of undesirable compounds and yet retain quality and tradition in such products.

2. Materials and Methods

2.1. Sample Preparation

Buđola samples (dry pork neck) were produced by a local meat processor. The raw materials used for the samples were domestically sourced, originating from the farms associated with the selected meat processor. The processing of raw materials and the production of samples were conducted according to traditional technology and subjected to the technological production procedures of the specified manufacturer. Before salting, each raw pork neck was weighed (around 1.7 kg). A mixture of nitrate and rock salt was manually added in an unspecified quantity. The meat was kept in the salt for seven days in a cooling chamber at 4 °C. After salting, the necks were rinsed with water and transferred for smoking and drying in a traditionally smokehouse, where they were drained and conditioned for approximately 20 h.

2.2. Smoking Conditions

When using the conventional smoking technique, pre-salted raw pork necks (three samples) were placed three meters away from an open fire. The process of smoking involved burning dry beech wood daily for the first six days (up to 8 h each day), and then every two or three days (2–3 h each session) for the following 14 days. This process continued for a total of 20 days under ambient conditions, with temperatures ranging from 3.7 to 11.3 °C (average 7.1 °C) and relative humidity between 62.1% and 91.2% (average 75.1%).

In the industrial setting, pre-salted pork necks (three samples) were kept in a ripening chamber for 13 days at an average temperature of 1 °C and a relative humidity of 60% until they lost about 15% of their initial weight. For smoking, a chamber from Mauting, Czech Republic, equipped with a heating plate smoke generator using beech sawdust, was utilized. The average temperature during smoking was 19.0 °C with a relative humidity of 74.4%. The pork necks were smoked for 4 h daily (8 sessions of 30 min each) over three days. During smoking, the temperature of the smoking materials was the same for both regimes, while the smoking time varied from 3 to 20 days.

Post-smoking, the pork necks were transferred to a ripening chamber (Mauting, Valtice, Czech Republic), where drying and ripening occurred at an average temperature of 15.0 °C and a relative humidity of 74.5%.

2.3. Sampling

Sampling was conducted at the end of the smoking process (on the 20th day for the traditional method and on the 3rd day for the industrial method). The production duration for both techniques (industrial and traditional) was 45 days. All sampling was performed in triplicate. Before determining PAH levels, the samples were stored in glass jars and kept in the dark at −30 °C until analysis, which was performed approximately one week after sampling. All analyses were conducted in triplicate. The sampling procedure is shown in

Table 1. Description of the conditions and variables applied to the tested samples.

Product	Smoking Conditions	Smoking Duration (Days)	Production Duration (Days)	Sampling Position
Buđola	traditional smoking	20	45	surface/inner
	industrial smoking	3	45	surface/inner

.

2.4. Calibration

Standard solutions of PAHs were produced using a blend of 16 PAHs (NA—naphthalene, AL—acenaphthylene, AN—acenaphthene, FL—fluorene, PHE—phenanthrene, ANT—anthracene (Ant), FLT—fluoranthene, PR—pyrene, BA—benz[a]anthracene, CHY—chrysene, BBF—benzo[b]fluoranthene, BKF—benzo[k]fluoranthene, BP—benzo[a]pyrene, IP—indeno[1,2,3-cd]pyrene, DAH—dibenz [a,h]anthracene and BGIH—benzo[ghi]perylene) (Ultra Scientific, North Kingstown, RI, USA) at a concentration of 500 ± 0.2 μg·mL⁻¹. To mitigate matrix effects, calibration was conducted with a matrix sample. The retention times of the peaks and target ions obtained from the standard solution of PAHs served as a base point for PAH determination in samples.

2.4.1. Sample Preparation for the Analyses

The samples were prepared using the QuEChERS assay, a quick, easy, effective, robust, and safe method of sample preparation, adapted from the official AOAC 2007.01 method for extraction and cleanup, as described by Mastanjević et al., 2020 [11]. This method involves extraction with acetonitrile (ACN Sigma-Aldrich, St. Louis, MI, USA) in the presence of anhydrous magnesium sulfate (MgSO₄; Merck, Darmstadt, Germany) and anhydrous sodium acetate (CH₃COONa; Merck, Darmstadt, Germany). It has already been applied to smoked meat products. For analysis, 3 g of the meat product sample was placed in a 50 mL centrifuge tube, to which 3 mL of ultrapure water and 3 mL of acetonitrile (ACN, Sigma-Aldrich, St. Louis, MO, USA) were added. The mixture is vortexed for 1 min, then 3 g of MgSO₄ (Merck, Darmstadt, Germany) and 1 g of NaAc were added. After another minute of vortexing, the mixture was centrifuged at 3000 RPM for 5 min at room temperature. The upper layer (1 mL) was transferred to a dSPE tube containing 150 mg MgSO₄, 50 mg PSA (Merck, Darmstadt, Germany), and 50 mg C18 (Merck, Darmstadt, Germany) vortexed for 60 s, and then centrifuged at 4000 RPM for 5 min at room temperature. Subsequently, 0.5 mL of the upper layer was transferred to a vial. Finally, the sample was evaporated to dryness under a stream of nitrogen and reconstituted with 0.5 mL n-hexane. The prepared sample was then ready for analysis on a gas chromatograph with mass spectrometry (GC-MS, Agilent 7890B/5977A, Santa Clara, CA, USA). In GC-MS, 4 mL of the sample was injected in splitless mode at 290 °C, using an Agilent HP-5 ms column (30 m × 0.25 µm), with helium as the mobile phase at a flow rate of 1.5 mL·min⁻¹. The temperature program was 55 °C for 1 min, then 25 °C·min⁻¹ to 320 °C, with a hold time of 3 min.

2.4.2. GC-MS

The GC-MS parameters were adjusted according to the methodology of Petrović et al. (2019) [17]. A DB-5MS column (30 m × 0.25 μm × 0.25 mm; Agilent J&W, Santa Clara, CA, USA) was employed for the separation of PAH molecules. A 4 mL sample was injected without splitting at a pressure of 11.36 psi and a carrier gas flow rate of 1.2 mL/min. Target and qualification quantities were determined by injecting a PAH standard mixture under the same conditions. Scanning was performed in the m/z range of 60–500. Standard solutions were prepared in control sample extracts to reduce matrix effects. PAH quantification was performed using the SIM mode, and the data were processed with a Mass Hunter software 10.2 SRI (G6845-10004). The method was calibrated in the range of 0.005 to 0.1 μg·kg⁻¹, with determination coefficients (r²) above 0.99. The analysis was conducted using an Agilent 7890B/5977A gas chromatograph-mass detector (GC-MSD). The injection temperature was 280 °C, and the injection volume was 4 μL. The column temperature was programmed to 50 °C (0.4 min), then increased to 195 °C (25 °C·min⁻¹, 1.5 min), then to 265 °C (8 °C·min⁻¹), and finally to 315 °C (20 °C·min⁻¹, 1.25 min). The MSD temperature was set at 280 °C. Peaks verification was conducted by comparing retention times and target ions. PAHs were not found in the blank samples.

2.4.3. Method Validation

The method for determining PAHs was adapted according to the accredited ISO 17025 method [18]. A sample with PAH concentrations below the detection limit was used for validation. The method’s performance criteria are aligned with SANTE/11312/2021 [19]. Four PAH compounds (BP, BA, BBF, and CHY) were analyzed according to these criteria. Validation includes the assessment of precision, repeatability, accuracy, linearity, LOQ, LOD, and uncertainty. Precision was evaluated using smoked meat enriched with PAHs (50.0 μg·kg⁻¹, n = 20). Accuracy was calculated based on recovery values. The detector’s linearity was tested in the range of 5 to 500 μg·kg⁻¹ and was satisfactory. The LOD values (0.29 to 0.5 μg·kg⁻¹) and LOQ values (1.05–2 μg·kg⁻¹) (Table S1) were slightly higher than the prescribed levels, Regulation No. 836/2011.

2.5. Statistics

The experimentally obtained data were processed using analysis of variance (ANOVA) and Fisher’s least significant difference (LSD) test, with statistical significance set at p < 0.05. Statistical analysis was performed using Statistica 12.7 software (2015, StatSoft Inc., Tulsa, OK, USA) and Microsoft Office Excel 2021 (Microsoft).

3. Results and Discussion

Of the 16 PAHs investigated, the raw material for producing “Buđola” (pork neck) contained only light PAHs (NP, FL, and ANT). ANT had the highest concentration (15.72 μg·kg⁻¹), followed by NP (11.23 μg·kg⁻¹) and FL with 6.31 μg·kg⁻¹. The remaining PAHs analyzed were below the quantification limit. These results are consistent with previously published studies on similar products [11,20]. Ref. [21] suggest that the presence of PAHs in animal tissues is due to environmental pollution. Consequently, the PAHs detected in the raw pork meat in this study can be linked to feed contamination.

The results of the individual concentrations of 16 PAHs and the total concentrations of PAH4 and PAH16 in dry-cured pork neck (Buđola), smoked traditionally and industrially (on the 3rd and 20th day of smoking) are shown in

Table 2. PAH concentrations (μg·kg⁻¹) in dry-cured pork neck (Buđola) at the end of smoking phase.

PAH	Traditional Smoking Methods		Industrial Smoking Methods
	Surface	Inner	Surface	Inner
NA	82.98 b ± 27.22	20.39 a ± 0.05	32.56 a ± 9.17	27.07 a ± 5.23
AL	549.73 b ± 77.57	19.01 a ± 3.83	17.99 a ± 4.55	-
AN	-	-	-	-
FL	339.19 b ± 61.21	13.05 a ± 3.88	-	-
ANT	207.99 b ± 49.77	8.02 a ± 1.99	-	-
PHE	839.44 b ± 165.34	40.08 a ± 9.88	-	-
FLT	69.67 b ± 15.99	6.52 a ± 0.78	-	-
BA	14.99 b ± 3.88	14.01 b ± 4.04	-	-
PR	48.03 b ± 11.22	3.03 b ± 0.61	-	-
CHY	-	-	-	-
BBF	1.49 b ± 0.22	0.55 a ± 0.10	-	-
BKF	3.99 c ± 0.39	3.18 b ± 0.16	-	-
BP	-	-	-	-
DAH	-	-	-	-
BGIH	-	-	-	-
IP	-	-	-	-
∑ PAH4	16.48 c ± 1.11	14.56 b ± 0.88	-	-
∑ PAH16	2157.50 d ± 99.72	127.84 c ± 6.22	50.55 b ± 3.10	27.07 a ± 5.23

The presented results are the mean value of nine replicates ± standard deviation; values within a row with the same letter (a–d) are not statistically different (p < 0.05); - below the limit of quantification (LOQ).

. The results are presented as the mean values with statistically significant differences determined at a confidence level of p < 0.05. Significant differences were found between all four groups of smoked dry-cured pork neck (traditional smoking—surface, traditional smoking—center, industrial smoking—surface, and industrial smoking—center).

In this research, the existence of 10 out of 16 investigated PAHs was confirmed in traditionally smoked pork neck (“Buđola”). On the other hand, in the industrial smoking samples, the presence of only two PAHs was determined. These results, which show the dominance of light PAHs, are consistent with previous studies on PAH contamination in smoked meat products [11,21,22].

The determined PAHs at the end of the smoking phase were as follows: NA (20.39–82.98 g·kg⁻¹), AL (549.73–18.50 μg·kg⁻¹), FL (339.19 μg·kg⁻¹ < LOQ), AN (207.99 μg·kg⁻¹ < LOQ), PHE (839.44 μg·kg⁻¹ < LOQ), FLT (69.67 μg·kg⁻¹ <LOQ), BA (14.99 μg·kg⁻¹ < LOQ), PR (48.03 μg·kg⁻¹ < LOQ), BBF (1.49 μg·kg⁻¹ < LOQ), and BKF (3.99 μg·kg⁻¹ < LOQ). Other investigated PAHs were below the limit of quantification. A statistically significant difference (p < 0.05) was found in the content of each individual PAH between the traditionally and industrially smoked samples, especially when comparing the surface layer, where the differences were very large. Comparing the internal samples of the traditional production with the internal and external samples of industrial production, no statistically significant differences were found. It is evident that PAHs are mostly retained on the surface layer, which also had higher values in industrial smoking compared to the inner layer, but the differences in concentrations were not as extreme as in traditional production.

The BP content in the all investigated samples, both traditionally and industrially smoked, was below the quantification limit. The BP values obtained in this study are lower than the average values obtained in previous research [5,8,9,10,15,16,17,23], but in accordance with the latest research on smoked meat products from Serbia [24]. The differences in BP levels can be linked to the traditional smoking methods, which vary by geographical region and the type of meat product. The total content of 16 US-EPA PAHs in dry-cured pork neck (“Buđola”) at the end of smoking phase was in the range from 2157.50 μg·kg⁻¹ (traditional smoking-surface) to 27.07 μg·kg⁻¹ (industrial smoking-inner), with significant differences (p < 0.05) between all investigated groups. These high levels of PAH are seldom observed, but they align with those found in smoking practices under uncontrolled technological conditions, common in households and developing countries [20,25]. Samples of the traditional smoked group were smoked around 90 h with 3 m of distance between the fire and samples, while the samples of the industrial smoked group were smoked for only 12 h. The longer smoking time resulted in higher contents of 16 US-EPA PAHs. The smoking duration of 3 days (8 h per day) can be considered optimal for dry-cured Buđola from the Herzegovina region, from a PAH viewpoint. The content of PAH4 at the end of the smoking phase was in the range from 16.48 μg·kg⁻¹ (traditional) to <LOQ (industrial smoking-surface and inner), with significant differences (p < 0.05) between the traditional and industrial sample groups.

Considering the data shown, several of the PAH species were either undetectable or present below the LOQ in samples from both the traditional and industrial smoking methods, as indicated by the dashes (“-”). These results indicate the variation in PAHs according to the smoking technique and the specific conditions the meat was subjected to during smoking. The undetectable or below-LOQ PAHs were as follows: AN (Anthracene), CHY (Chrysene), BP (Benzo[a]pyrene), DAH (Dibenzo[a,h]anthracene), BGIH (Benzo[ghi]perylene), and IP (Indeno[1,2,3-cd]pyrene). It is likely that none of these PAH compounds was detected during conventional and industrial smoking due to their relatively lower volatility or due to these conditions not fulfilling the requirements for either temperature or time of smoking. In many cases, these PAHs would be formed at higher temperatures; their very absence might indicate that the temperature of the smoke did not rise to the level generally expected to generate them. For example, benzo[a]pyrene (BP), a common indicator of PAH contamination, was below the limit of detection and thus could testify that either the smoking temperatures or types of wood used were controlled in order not to generate it. Acenaphthene, Fluoranthene, Fluorene, Pyrene, and Phenanthrene appeared only on the surface of traditionally smoked Buđola. These compounds did not appear in samples obtained with industrial smoking. Usually, smoking in industry is performed under more controlled conditions and probably at lower temperatures, which may reduce the formation of these PAHs. Additionally, it is foreseen that the general formation of PAHs through industrial methods of smoking is reduced by the use of liquid smoke or filtered smoke that minimizes deposition of PAHs. The PAHs Benzo[b]fluoranthene (BBF) and Benzo[k]fluoranthene (BKF) appeared only in low concentrations in traditionally smoked samples. Higher concentrations were found on the surface compared to inside the samples. However, they were below the LOQ in the industrially smoked Buđola. BBF and BKF are high molecular weight PAHs usually formed during prolonged or intense smoking, thus indicating that traditional smoking provides more time for these PAHs to form, especially on the surface of the product, while industrial methods do manage to effectively prevent accumulation. Considering the differences by method, there were considerably higher concentrations of PAHs in traditional smoking due to prolonged exposure to unfiltered smoke, as evidenced by the fact that surface Buđola was more burdened than the other sample sites. The presence of several PAHs (naphthalene (NA), acenaphthylene (AL), and phenanthrene (PHE) in traditional smoking that were absent in industrial smoked samples further underlines the role of uncontrolled, open-fire smoking in increasing PAH formation. In contrast, much lower general levels of PAHs characterize industrial smoking methods. The reduction in PAH levels can be achieved with better control over smoking conditions, either by purifying smoke or using alternative methods such as liquid smoke, where there will not be as many PAHs formed. This is supported by the significantly lower ∑PAH16 in industrially smoked “Buđola” (50.55 ± 3.10) than in the traditionally smoked samples (2157.50 ± 99.72). Basically, this means that the industrial smoking method results in an almost negligible level of PAHs in the inner layers of the meat. It is observed that some of the PAHs, particularly those of high molecular weight, are more concentrated in traditional smoking, especially on the surface. By adopting methods from industry, safer products are produced with a minimal formation of PAHs or deposition in both the surface and inner layers.

The concentrations of 16 individual PAHs and the total concentrations of PAH4 and PAH16 in “Buđola” at the end of the production period (45th day) are shown in

Table 3. PAH concentrations (μg·kg⁻¹) in dry-cured pork neck (Buđola) at the end of production.

PAH	Traditional Smoking Methods		Industrial Smoking Methods
	Surface	Inner	Surface	Inner
NA	208.05 b ± 49.69	23.42 a ± 6.93	3.99 a ± 1.75	4.32 a ± 0.33
AL	633.85 b ± 128.26	45.02 a ± 11.28	23.05 a ± 1.99	-
AN	-	-	-	-
FL	360.59 b ± 74.68	18.78 a ± 5.57	-	-
ANT	1644.81 b ± 181.45	76.60 a ± 11.92	-	-
PHE	459.99 b ± 47.82	12.01 a ± 1.97	-	-
FLT	140.77 b ± 17.89	8.03 a ± 1.90	-	-
BA	22.75 b ± 4.08	19.04 a ± 0.99	-	-
PR	107.95 b ± 21.88	5.99 a ± 2.07	-	-
CHY	-	-	-	-
BBF	3.05 c ± 0.23	2.10 b ± 0.28	-	-
BKF	6.02 c ± 1.27	5.11 b ± 0.78	-	-
BP	-	-	-	-
DAH	-	-	-	-
BGIH	-	-	-	-
IP	-	-	-	-
∑ PAH4	28.77 c ± 2.11	21.14 b ± 0.95	-	-
∑ PAH16	3587.83 d ± 130.77	186.10 c ± 8.98	27.04 b ± 1.87	4.32 a ± 0.33

The presented results are the mean values of nine replicates ± standard deviation; values within a row with the same letter (a–d) are not statistically different (p < 0.05); - below the limit of quantification (LOQ).

.

Similar to the results after the smoking phase, at the end of production, 10 (Na, AN, FL, AL, PHE, FLT, BA, PR, BBF, BKF) out of 16 PAHs were determined in the traditional smoked sample group, while in the industrial sample group, there were only two (NA, AL). The PAHs identified at the end of production were as follows: NA (208.05–3.99 μg·kg⁻¹), AL (633.85–23.05 μg·kg⁻¹), FL (360.59 μg·kg⁻¹ < LOQ), ANT (1644.81 μg·kg⁻¹ < LOQ), PHE (459.99 μg·kg⁻¹ < LOQ), FLT (140.77 μg·kg⁻¹ < LOQ), BA (22.75 μg·kg⁻¹ < LOQ), PR (107.95 μg·kg⁻¹ < LOQ), BBF (3.05 μg·kg⁻¹ < LOQ), and BKF (6.02 μg·kg⁻¹ < LOQ). The other investigated PAHs were below the limit of quantification. In traditional production, there was a noticeable increase in the concentrations of each individual PAH, both on the surface and in the inner layer. A statistically significant difference (p < 0.05) in the concentration of each individual PAH between the samples from traditional and industrial production was still found for the surface samples, while no statistically significant difference was found for the internal samples. The increase in PAH concentration in traditional production after the ripening period could be attributed to concentration due to dehydration. On the other hand, in industrial production, there was a decrease in the concentrations of detected PAHs, both for the surface and interior samples. This could be because only light, volatile PAHs were detected in industrial production. BP, at the end of production period, was still under the limit of quantification.

The total content of 16 US-EPA PAHs was in the range from 3587.83 μg·kg⁻¹ (traditional smoking—surface) to 4.32 μg·kg⁻¹ (industrial smoking—inner), with significant differences (p < 0.05) between all investigated groups. It is important to note that the total content of PAH16 after the ripening period in traditional production was up to 40% higher compared to the concentrations after the smoking phase. On the other hand, in industrial production, there was a decrease in the concentrations of PAH16 of up to 49%. These results indicate the importance of selecting the appropriate smoking process and method, as well as the duration of smoking, and how they can yield different outcomes in PAH16 concentrations. The content of PAH4 at the end of the ripening phase was in the range from 24.13 μg·kg⁻¹ (traditional smoking—surface) to <LOQ (industrial smoking—surface and inner), with significant differences (p < 0.05) between the traditional and industrial sample groups. In traditional production, due to dehydration, at the end of the ripening process, there was an increase in PAH4 concentrations by up to 29% compared to the concentrations after the smoking phase. In industrial production, PAH4 concentrations after the ripening process remained below the limit of quantification for both investigated sample groups (surface and inner). High levels of PAHs are associated with an increased risk of cancer. Therefore, the results suggest that, from a health perspective, excessive consumption of “Buđola” produced using traditional smoking methods may pose certain health risks. Although PAH4 and BP concentrations comply with the higher concentrations allowed for traditional products under regulatory criteria—EU Regulation 2023/915 (BaP < 5 μg/kg; PAH4 < 30 μg/kg)—the total PAH16 concentrations in traditional smoking are worryingly high, raising concerns about the safety of such products.

Similar results for PAH16 and PAH4 content in Portuguese traditional smoked meat products have been reported (PAH16: 877.37–2609.81 μg·kg⁻¹; PAH4: 3.47–6.94 μg·kg⁻¹) [21]. Also, similar results were obtained in traditional meat products from Cyprus [8] (PAH4: 5.9–15.2 μg·kg⁻¹) as well as in dry-cured meat products from Herzegovina [20] (PAH16: 145–2474 μg·kg⁻¹; PAH4: 12.7–32.5 μg·kg⁻¹). However, traditional meat products from Spain [9,10] (<100 μg·kg⁻¹), and Italy [26] (<100 μg·kg⁻¹), as well as sausages from Herzegovina [27] (<300 μg·kg⁻¹) showed lower amounts of PAH16 in relation to the findings of this study. The latest research on PAH content in traditionally smoked meat products from Serbia [24] show significantly lower values of PAH16 in relation to the findings of this study. (The total content of 16 US-EPA PAHs in dry-cured meat products was in the range from 99.73 μg·kg⁻¹ to 412.76 μg·kg⁻¹; in bacons, it was in the range from 36.43 μg·kg⁻¹ to 188.86 μg·kg⁻¹; and in dry fermented sausages, in the range from 47.23 μg·kg⁻¹ to 270.60 μg·kg⁻¹). Therefore, the shortened smoking process is warranted as it yields products with good sensory quality and reduced PAH compounds. These results could also be applied in the production of “Buđola” with the aim of reducing the PAH concentrations. The differences in PAH levels can be linked to the traditional smoking methods, which differ by region and type of meat. Factors such as temperature, humidity, wood type, smoke intensity, smoking duration, and meat type influence the PAH levels in traditional meat products [2,5,9,10,15,28,29].

In general, this study demonstrated that traditionally smoked samples exhibited the highest levels of the 16 polycyclic aromatic hydrocarbons (PAHs) identified by the US Environmental Protection Agency (EPA), particularly when the smoking process was more intense (20 days). One significant factor contributing to elevated PAH levels is the smoking technique. Additionally, the duration of smoking plays a crucial role; the longer the samples are smoked, the higher the PAH concentration. The results suggest that to reduce PAH levels in traditionally smoked Buđola, manufacturers should consider shortening the smoking duration. From a health perspective, industrially produced “Buđola” is safer for consumption than those meats smoked in uncontrolled conditions. This study indicates that it is not feasible to produce traditional Buđola with typical sensory characteristics and a lower content of PAH compounds (BP < 2 μg·kg⁻¹; PAH4 < 12 μg·kg⁻¹). Therefore, it is necessary for traditional products from Herzegovina to comply with the new regulatory criteria of the EU regulation (BP < 5 μg·kg⁻¹; PAH4 < 30 μg·kg⁻¹) [7].

4. Conclusions

The overall amounts of 16 US-EPA PAHs and PAH4 in Buđola were between 3587.83 μg·kg⁻¹ (traditional smoking) and 4.32 μg·kg⁻¹ (industrial smoking), and between 28.77 μg·kg⁻¹ (traditional smoking) and <LOQ (industrial smoking). These results suggest that to reduce PAH levels in traditionally produced smoked meat product Buđola from Herzegovina, producers should consider shortening the smoking process and modernizing open fire smoking methods, and also ensure their proper management. All the examined samples had BP contents lower than the limit of quantification. The PAH4 concentrations for the traditional production were higher than the set maximum value (BP < 2 μg·kg⁻¹; PAH4 < 12 μg·kg⁻¹), while concentrations in the industrial samples were under the limit of quantification. Such results indicate the need to apply the new regulatory criteria—EU Regulation 2023/915 (BP < 5 μg/kg; PAH4 < 30 μg/kg) to the traditional smoked Buđola from the Herzegovina region. To optimize the conditions for smoking traditionally smoked meat, with the aim of balancing safety and flavour, future research should focus on the investigating different types of wood, controlling the temperature and duration of smoking, and conducting sensory evaluations. Conducting sensory tests with consumers to assess the taste, aroma, and texture of smoked meat under various smoking conditions can provide valuable feedback for process optimization.