Development of a Method for Simultaneous Analysis of Allergenic Flavoring Agents in Cigarettes and Quantitative Risk Assessment for Consumer Safety
Abstract
:1. Introduction
2. Materials and Methods
2.1. Chemicals
2.2. Sample Preparation
2.3. Method Validation
2.4. GC-MS/MS Analysis
2.5. Statistical Analysis
2.6. Estimation of Inhalation Exposure from Allergenic Flavoring Agents among Cigarette Smokers
- C (μg/cigarette): content of allergen per cigarette
- N: average number of cigarettes smoked per day
- ED (years): exposure duration
- EF (days/years): exposure frequency
- IR (m3/day): daily inhalation rate
- AT (h): averaging time (ED × 365 days/year)
2.7. Risk Characterization
3. Results
3.1. Method Validation
3.2. Applicability of Analysis Method to Commercial Cigarettes
3.3. Comparison of Levels of Flavoring Agents between Non-Capsule and Capsule Cigarettes
3.4. Estimation of Inhalation Exposure and Risk Characterization
4. Discussion
5. Conclusions
Supplementary Materials
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Compound | Tobacco (n = 54) | Filter Tip (n = 54) | Capsule (n = 42) | |||||||||||||||
---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
N | Mean | Median | SD | Min | Max | N | Mean | Median | SD | Min | Max | N | Mean | Median | SD | Min | Max | |
D-Limonene | 7 | 8.50 | 3.02 | 10.93 | 0.33 | 30.49 | 11 | 8.85 | 1.24 | 14.68 | 0.26 | 45.62 | 40 | 265.07 | 30.87 | 379.35 | 0.43 | 1578.66 |
Linalool | 21 | 0.60 | 0.06 | 1.68 | 0.04 | 7.83 | 44 | 1.92 | 0.08 | 6.85 | 0.03 | 40.69 | 41 | 33.31 | 4.39 | 63.04 | 0.03 | 299.91 |
Methyl 2-octynoate | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Citral | 54 | 0.29 | 0.21 | 0.49 | 0.11 | 3.87 | 16 | 7.67 | 0.09 | 28.57 | 0.07 | 118.27 | 29 | 24.62 | 2.50 | 64.42 | 0.04 | 255.34 |
Citronellol | 0 | ND | - | - | - | - | 2 | 1.89 | 1.89 | 1.36 | 0.53 | 3.25 | 25 | 2.81 | 0.44 | 5.45 | 0.14 | 25.49 |
Geraniol | 0 | ND | - | - | - | - | 6 | 1.30 | 0.74 | 1.08 | 0.35 | 3.14 | 26 | 9.74 | 1.10 | 25.91 | 0.09 | 130.26 |
α-Isomethyl ionone | 12 | 0.02 | 0.02 | 0.00 | 0.02 | 0.03 | 8 | 0.03 | 0.02 | 0.01 | 0.02 | 0.05 | 1 | 0.02 | 0.02 | 0.00 | 0.02 | 0.02 |
Benzyl alcohol | 52 | 2.80 | 0.74 | 5.52 | 0.09 | 28.97 | 54 | 18.43 | 1.32 | 36.17 | 0.26 | 166.73 | 21 | 30.78 | 0.16 | 93.53 | 0.05 | 330.43 |
Hydroxycitronellal | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Methyl eugenol | 0 | ND | - | - | - | - | 1 | 0.03 | 0.03 | 0.00 | 0.03 | 0.03 | 12 | 0.06 | 0.02 | 0.09 | 0.01 | 0.32 |
Cinnamaldehyde | 0 | ND | - | - | - | - | 7 | 0.36 | 0.14 | 0.40 | 0.05 | 1.25 | 10 | 43.56 | 0.05 | 69.30 | 0.01 | 182.40 |
Lilial | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Eugenol | 4 | 0.14 | 0.12 | 0.06 | 0.08 | 0.23 | 1 | 1.00 | 1.00 | 0.00 | 1.00 | 1.00 | 27 | 0.24 | 0.24 | 0.17 | 0.03 | 0.74 |
α-Amylcinnamaldehyde | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Anise alcohol | 4 | 0.37 | 0.33 | 0.14 | 0.22 | 0.58 | 2 | 0.46 | 0.46 | 0.05 | 0.41 | 0.51 | 0 | ND | - | - | - | - |
Cinnamyl alcohol | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 3 | 0.25 | 0.31 | 0.13 | 0.07 | 0.36 |
Isoeugenol | 5 | 0.34 | 0.26 | 0.18 | 0.17 | 0.66 | 0 | ND | - | - | - | - | 5 | 0.37 | 0.07 | 0.43 | 0.01 | 1.03 |
α-Hexylcinnamaldehyde | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Farnesol | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 2 | 0.22 | 0.22 | 0.00 | 0.22 | 0.22 |
Coumarin | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
HICC | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
α-Amylcinnamyl alcohol | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Benzyl benzoate | 31 | 0.41 | 0.06 | 1.12 | 0.03 | 5.18 | 9 | 0.18 | 0.08 | 0.14 | 0.05 | 0.45 | 7 | 0.20 | 0.12 | 0.14 | 0.02 | 0.38 |
Benzyl salicylate | 2 | 0.51 | 0.51 | 0.04 | 0.47 | 0.56 | 0 | ND | - | - | - | - | 0 | ND | - | - | - | - |
Benzyl cinnamate | 0 | ND | - | - | - | - | 1 | 1.18 | 1.18 | 0.00 | 1.18 | 1.18 | 6 | 2.08 | 0.04 | 2.91 | 0.02 | 6.32 |
Menthol | 53 | 191.07 | 1.34 | 448.81 | 0.05 | 1868.14 | 53 | 417.05 | 2.39 | 863.24 | 0.11 | 3011.88 | 42 | 1518.22 | 1378.95 | 450.78 | 689.47 | 2419.50 |
Compound | N | Kruskal-Wallis Test | Pairwise Comparisons Using Dunn-Bonferroni Test | ||||
---|---|---|---|---|---|---|---|
H | df | p-Value | Mean Difference | p-Value | |||
All analytes | 757 | 56.721 | 2 | <0.001 *** | tobacco-filter tip | −3.325 | 0.003 ** |
tobacco-capsule | −7.511 | <0.001 *** | |||||
filter tip-capsule | −3.770 | <0.001 *** | |||||
D-Limonene | 58 | 17.768 | 2 | <0.001 *** | tobacco-filter tip | −0.336 | 1.000 |
tobacco-capsule | −2.669 | 0.023 * | |||||
filter tip-capsule | −3.688 | 0.001 ** | |||||
Linalool | 106 | 50.156 | 2 | <0.001 *** | tobacco-filter tip | −0.967 | 1.000 |
tobacco-capsule | −5.861 | <0.001 *** | |||||
filter tip-capsule | −6.064 | <0.001 *** | |||||
Citral | 99 | 28.855 | 2 | <0.001 *** | tobacco-filter tip | −3.308 | 0.006 ** |
tobacco-capsule | −3.347 | 0.002 ** | |||||
filter tip-capsule | −5.293 | <0.001 *** | |||||
Benzyl alcohol | 127 | 25.216 | 2 | <0.001 *** | tobacco-filter tip | −2.981 | 0.009 ** |
tobacco-capsule | −2.582 | 0.029 * | |||||
filter tip-capsule | −4.848 | <0.001 *** | |||||
Menthol | 148 | 62.913 | 2 | <0.001 *** | tobacco-filter tip | −1.994 | 0.138 |
tobacco-capsule | −7.713 | <0.001 *** | |||||
filter tip-capsule | −5.838 | <0.001 *** |
Compound | Non-Capsule Cigarette (n = 24) | Capsule Cigarette (n = 30) | ||
---|---|---|---|---|
Tobacco | Filter Tip | Tobacco | Filter Tip | |
D-Limonene | ND (0) | 0.47 ± 0.31 (4) | 8.50 ± 10.93 (7) | 13.64 ± 16.60 (7) |
Linalool | 0.05 ± 0.01 (8) | 0.07 ± 0.03 (17) | 0.94 ± 2.06 (13) | 3.08 ± 8.54 (37) |
Methyl 2-octynoate | ND (0) | ND (0) | ND (0) | ND (0) |
Citral | 0.22 ± 0.06 (24) | 0.10 ± 0.02 (10) | 0.35 ± 0.66 (30) | 20.30 ± 43.83 (6) |
Citronellol | ND (0) | ND (0) | ND (0) | 1.89 ± 1.36 (2) |
Geraniol | ND (0) | 0.57 (1) | ND (0) | 1.45 ± 1.13 (5) |
α-Isomethyl ionone | 0.02 ± 0.00 (3) | ND (0) | 0.02 ± 0.00 (9) | 0.03 ± 0.01 (8) |
Benzyl alcohol | 3.63 ± 7.14 (22) | 8.40 ± 13.27 (24) | 2.19 ± 3.81 (30) | 26.46 ± 45.49 (30) |
Hydroxycitronellal | ND (0) | ND (0) | ND (0) | ND (0) |
Methyl eugenol | ND (0) | ND (0) | ND (0) | 0.03 (1) |
Cinnamaldehyde | ND (0) | ND (0) | ND (0) | 0.36 ± 0.40 (7) |
Lilial | ND (0) | ND (0) | ND (0) | ND (0) |
Eugenol | 0.11 ± 0.03 (2) | ND (0) | 0.16 ± 0.07 (2) | 1.00 (1) |
α-Amylcinnamaldehyde | ND (0) | ND (0) | ND (0) | ND (0) |
Anise alcohol | 0.41 (1) | ND (0) | 0.35 ± 0.16 (3) | 0.46 ± 0.05 (2) |
Cinnamyl alcohol | ND (0) | ND (0) | ND (0) | ND (0) |
Isoeugenol | 0.22 ± 0.04 (3) | ND (0) | 0.53 ± 0.14 (2) | ND (0) |
α-Hexylcinnamaldehyde | ND (0) | ND (0) | ND (0) | ND (0) |
Farnesol | ND (0) | ND (0) | ND (0) | ND (0) |
Coumarin | ND (0) | ND (0) | ND (0) | ND (0) |
HICC | ND (0) | ND (0) | ND (0) | ND (0) |
α-Amylcinnamyl alcohol | ND (0) | ND (0) | ND (0) | ND (0) |
Benzyl benzoate | 1.08 ± 1.90 (9) | 0.06 (1) | 0.13 ± 0.17 (22) | 0.19 ± 0.14 (8) |
Benzyl salicylate | 0.51 ± 0.04 (2) | ND (0) | ND (0) | ND (0) |
Benzyl cinnamate | ND (0) | ND (0) | ND (0) | 1.18 (1) |
Menthol | 0.75 ± 0.77 (23) | 1.35 ± 1.04 (23) | 336.98 ± 553.89 (30) | 735.76 ± 1040.40 (30) |
Compound | Category | Tobacco (n = 54) | Filter (n = 54) | ||||||||
---|---|---|---|---|---|---|---|---|---|---|---|
N | Mean | Sum | Mann-Whitney U | p-Value | N | Mean | Sum | Mann-Whitney U | p-Value | ||
All analytes | Non-capsule | 97 | 119.93 | 11,633 | 6880 | 0.583 | 80 | 93.31 | 7465 | 4225 | 0.008 ** |
Capsule | 148 | 125.01 | 18,502 | 135 | 116.70 | 15,755 | |||||
D-Limonene | Non-capsule | 0 | 0.00 | 0 | - | - | 4 | 2.75 | 11 | 1 | 0.014 * |
Capsule | 7 | 4.00 | 28 | 7 | 7.86 | 55 | |||||
Linalool | Non-capsule | 8 | 6.38 | 51 | 15 | 0.007 ** | 17 | 14.76 | 251 | 98 | 0.002 ** |
Capsule | 13 | 13.85 | 180 | 27 | 27.37 | 739 | |||||
Citral | Non-capsule | 24 | 25.88 | 621 | 321 | 0.497 | 10 | 8.30 | 83 | 28 | 0.828 |
Capsule | 30 | 28.80 | 864 | 6 | 8.83 | 53 | |||||
α-Isomethyl ionone | Non-capsule | 3 | 2.67 | 8 | 2 | 0.033 * | 0 | 0.00 | 0 | - | - |
Capsule | 9 | 7.78 | 70 | 8 | 4.50 | 36 | |||||
Benzyl alcohol | Non-capsule | 22 | 30.00 | 660 | 253 | 0.154 | 24 | 22.46 | 539 | 239 | 0.035 * |
Capsule | 30 | 23.93 | 718 | 30 | 31.53 | 946 | |||||
Benzyl benzoate | Non-capsule | 9 | 21.22 | 191 | 52 | 0.041 * | 1 | 2.00 | 2 | 1 | 0.245 |
Capsule | 22 | 13.86 | 305 | 8 | 5.38 | 43 | |||||
Menthol | Non-capsule | 23 | 18.26 | 420 | 144 | <0.001 *** | 23 | 17.30 | 398 | 122 | <0.001 *** |
Capsule | 30 | 33.70 | 1011 | 30 | 34.43 | 1033 |
Compound | DNEL a (mg/m3) | Average | Maximum | ||||
---|---|---|---|---|---|---|---|
Content (μg/Cigarette) | Exposure (mg/m3) | RCRb | Content (μg/Cigarette) | Exposure (mg/m3) | RCR | ||
D-Limonene | 16.6 | 119.47 | 0.11067 | 6.7 × 10−3 | 818.21 | 0.75792 | 4.6 × 10−2 |
Linalool | 0.7 | 23.22 | 0.02151 | 3.1 × 10−2 | 301.86 | 0.27962 | 4.0 × 10−1 |
Citral | 2.7 | 15.12 | 0.01400 | 5.2 × 10−3 | 255.67 | 0.23683 | 8.8 × 10−2 |
Citronellol | 47.8 | 1.60 | 0.00149 | 3.1 × 10−5 | 26.15 | 0.02422 | 5.1 × 10−4 |
Geraniol | 47.8 | 4.27 | 0.00396 | 8.3 × 10−5 | 130.58 | 0.12096 | 2.5 × 10−3 |
α-Isomethyl ionone | 1.45 | 0.04 | 0.00004 | 2.6 × 10−5 | 0.08 | 0.00008 | 5.3 × 10−5 |
Benzyl alcohol | 5.4 | 33.10 | 0.03066 | 5.7 × 10−3 | 474.41 | 0.43945 | 8.1 × 10−2 |
Methyl eugenol | 1.74 | 0.05 | 0.00005 | 2.6 × 10−5 | 0.35 | 0.00033 | 1.9 × 10−4 |
Cinnamaldehyde | 1.09 | 8.15 | 0.00755 | 6.9 × 10−3 | 182.95 | 0.16947 | 1.6 × 10−1 |
Eugenol | 5.22 | 0.27 | 0.00025 | 4.8 × 10−5 | 1.38 | 0.00128 | 2.5 × 10−4 |
Anise alcohol | 0.37 | 0.33 | 0.00031 | 8.3 × 10−4 | 1.16 | 0.00107 | 2.9 × 10−3 |
Cinnamyl alcohol | 0.465 | 0.09 | 0.00008 | 1.8 × 10−4 | 0.43 | 0.00040 | 8.5 × 10−4 |
Isoeugenol | 5.22 | 0.33 | 0.00031 | 5.9 × 10−5 | 1.27 | 0.00118 | 2.3 × 10−4 |
Farnesol | 0.457 | 0.86 | 0.00080 | 1.7 × 10−3 | 1.12 | 0.00103 | 2.3 × 10−3 |
Benzyl benzoate | 1.25 | 0.33 | 0.00031 | 2.5 × 10−4 | 5.24 | 0.00485 | 3.9 × 10−3 |
Benzyl salicylate | 1.37 | 0.61 | 0.00057 | 4.1 × 10−4 | 0.82 | 0.00076 | 5.5 × 10−4 |
Benzyl cinnamate | 1.74 | 0.33 | 0.00030 | 1.7 × 10−4 | 6.41 | 0.00593 | 3.4 × 10−3 |
Menthol | 8.17 | 1565.01 | 1.44969 | 1.8 × 10−1 | 7870.83 | 7.29087 | 8.9 × 10−1 |
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Jang, D.Y.; Kim, H.S.; Pack, E.C.; Koo, Y.J.; Lim, K.M.; Choi, D.W. Development of a Method for Simultaneous Analysis of Allergenic Flavoring Agents in Cigarettes and Quantitative Risk Assessment for Consumer Safety. Toxics 2021, 9, 87. https://doi.org/10.3390/toxics9040087
Jang DY, Kim HS, Pack EC, Koo YJ, Lim KM, Choi DW. Development of a Method for Simultaneous Analysis of Allergenic Flavoring Agents in Cigarettes and Quantitative Risk Assessment for Consumer Safety. Toxics. 2021; 9(4):87. https://doi.org/10.3390/toxics9040087
Chicago/Turabian StyleJang, Dae Yong, Hyung Soo Kim, Eun Chul Pack, Ye Ji Koo, Kyung Min Lim, and Dal Woong Choi. 2021. "Development of a Method for Simultaneous Analysis of Allergenic Flavoring Agents in Cigarettes and Quantitative Risk Assessment for Consumer Safety" Toxics 9, no. 4: 87. https://doi.org/10.3390/toxics9040087
APA StyleJang, D. Y., Kim, H. S., Pack, E. C., Koo, Y. J., Lim, K. M., & Choi, D. W. (2021). Development of a Method for Simultaneous Analysis of Allergenic Flavoring Agents in Cigarettes and Quantitative Risk Assessment for Consumer Safety. Toxics, 9(4), 87. https://doi.org/10.3390/toxics9040087