Pesticides Contamination of Cereals and Legumes: Monitoring of Samples Marketed in Italy as a Contribution to Risk Assessment
Abstract
:Featured Application
Abstract
1. Introduction
2. Materials and Methods
2.1. Chemicals
2.2. Sampling and Sample Preparation
2.3. Gas Chromatography/Mass Spectrometry Analyses
2.4. Risk Exposure
3. Results
3.1. Method Validation
3.2. Contamination Grade by Pesticide Residues in Cereals and Legumes
3.3. Risk Exposure Study
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
- Tadeo, J.L. (Ed.) Analysis of Pesticides in Food and Environmental Samples, 2nd ed.; Boca Raton: Taylor & Francis, a CRC Title, Part of the Taylor & Francis Imprint, a Member of the Taylor & Francis Group, the Academic Division of T&F Informa, plc; CRC Press: Boca Raton, FL, USA, 2019; ISBN 978-1-351-04708-1. [Google Scholar]
- Wesseling, C.; Keifer, M.; Ahlbom, A.; McConnell, R.; Moon, J.-D.; Rosenstock, L.; Hogstedt, C. Long-term Neurobehavioral Effects of Mild Poisonings with Organophosphate and n-Methyl Carbamate Pesticides among Banana Workers. Int. J. Occup. Environ. Health 2002, 8, 27–34. [Google Scholar] [CrossRef]
- Anadón, A.; Martínez-Larrañaga, M.R.; Martínez, M.A. Use and abuse of pyrethrins and synthetic pyrethroids in veterinary medicine. Vet. J. 2009, 182, 7–20. [Google Scholar] [CrossRef]
- EU Pesticides Database (v.2.2) Search Pesticide Residues. Available online: https://ec.europa.eu/food/plant/pesticides/eu-pesticides-database/mrls/?event=search.pr (accessed on 24 May 2021).
- Likas, D.T.; Tsiropoulos, N.G.; Miliadis, G.E. Rapid gas chromatographic method for the determination of famoxadone, trifloxystrobin and fenhexamid residues in tomato, grape and wine samples. J. Chromatogr. A 2007, 1150, 208–214. [Google Scholar] [CrossRef]
- Nardelli, V.; Casamassima, F.; Gesualdo, G.; Li, D.; Marchesiello, W.M.V.; Nardiello, D.; Quinto, M. Sensitive Screening Method for Determination of Pyrethroids in Chicken Eggs and Various Meat Samples by Gas Chromatography and Electron Capture Detection. J. Agric. Food Chem. 2018, 66, 10267–10273. [Google Scholar] [CrossRef] [PubMed]
- Lobato, A.; Fernandes, V.C.; Pacheco, J.G.; Delerue-Matos, C.; Gonçalves, L.M. Organochlorine pesticide analysis in milk by gas-diffusion microextraction with gas chromatography-electron capture detection and confirmation by mass spectrometry. J. Chromatogr. A 2021, 1636, 461797. [Google Scholar] [CrossRef]
- Lehotay, S.J.; Son, K.A.; Kwon, H.; Koesukwiwat, U.; Fu, W.; Mastovska, K.; Hoh, E.; Leepipatpiboon, N. Comparison of QuEChERS sample preparation methods for the analysis of pesticide residues in fruits and vegetables. J. Chromatogr. A 2010, 1217, 2548–2560. [Google Scholar] [CrossRef]
- Cunha, S.C.; Fernandes, J.O. Multipesticide residue analysis in maize combining acetonitrile-based extraction with dispersive liquid–liquid microextraction followed by gas chromatography–mass spectrometry. J. Chromatogr. A 2011, 1218, 7748–7757. [Google Scholar] [CrossRef] [PubMed]
- Marletta, L.; Lucarini, M.; Ruggeri, S.; Carnovale, E. Food Composition Databases in Italy: Problems and Perspectives. J. Food Compos. Anal. 2000, 13, 611–618. [Google Scholar] [CrossRef]
- Marletta, L.; Camilli, E.; Turrini, A.; Scardella, P.; Spada, R.; Piombo, L.; Khokhar, S.; Finglas, P.; Carnovale, E. The nutritional composition of selected ethnic foods consumed in Italy. Nutr. Bull. 2010, 35, 350–356. [Google Scholar] [CrossRef]
- European Commission. Commission Directive 2011/81/EU of 20 September 2011 Amending Directive 98/8/EC of the European Parliament and of the Council to Include Deltamethrin as an Active Substance in Annex I Thereto. Off. J. Eur. Union 2011, L243, 16–18. [Google Scholar]
- European Commission. Commission Directive 2013/41/EU of 18 July 2013 Amending Directive 98/8/EC of the European Parliament and of the Council to Include 1R-Trans Phenothrin as an Active Substance in Annex I TheretoText with EEA Relevance. Off. J. Eur. Union 2013, 18–20. [Google Scholar]
- European Food Safety Authority. Conclusion on the peer review of the pesticide risk assessment of the active substance esfenvalerate. EFSA J. 2014, 12, 3873. [Google Scholar] [CrossRef] [Green Version]
- European Food Safety Authority Public Consultation on the Active Substance Pirimiphos-Methyl. Available online: https://www.efsa.europa.eu/en/consultations/call/180212 (accessed on 5 May 2021).
- European Commission. European Commission Regulation (EU) No 528/2012 Concerning the Making Available on the Market and Use of Biocidal Products—Evaluation of Active Substances, Assessment Report: Cyfluthrin Product-Type 18 (Insecticides, Acaricides and Products to Control Other Arthropods). Off. J. Eur. Union 2018, L1-167. [Google Scholar]
- European Food Safety Authority (EFSA); Brancato, A.; Brocca, D.; De Lentdecker, C.; Erdos, Z.; Ferreira, L.; Greco, L.; Jarrah, S.; Kardassi, D.; Leuschner, R.; et al. Modification of the existing maximum residue level for deltamethrin in kale. EFS2 J. 2018, 16, e05153. [Google Scholar] [CrossRef] [Green Version]
- European Food Safety Authority (EFSA); Arena, M.; Auteri, D.; Barmaz, S.; Brancato, A.; Brocca, D.; Bura, L.; Carrasco Cabrera, L.; Chiusolo, A.; Civitella, C.; et al. Peer Review of the Pesticide Risk Assessment of the Active Substance Cypermethrin. EFSA J. 2018, 16, e05403. [Google Scholar] [CrossRef] [Green Version]
- European Food Safety Authority (EFSA). Statement on the available outcomes of the human health assessment in the context of the pesticides peer review of the active substance chlorpyrifos. EFSA J. 2019, 17, e05809. [Google Scholar] [CrossRef]
- EFSA Scientific Committee. Guidance on selected default values to be used by the EFSA Scientific Committee, Scientific Panels and Units in the absence of actual measured data. EFSA J. 2012, 10, 2579. [Google Scholar] [CrossRef]
- Leclercq, C.; Arcella, D.; Piccinelli, R.; Sette, S.; Le Donne, C.; Turrini, A.; on behalf of the INRAN-SCAI 2005–06 Study Group. The Italian National Food Consumption Survey INRAN-SCAI 2005–06: Main results in terms of food consumption. Public Health Nutr. 2009, 12, 2504–2532. [Google Scholar] [CrossRef] [PubMed] [Green Version]
- Rizzi, A. Inferenza Statistica; UTET Università: Novara, Italy, 1992; ISBN 88-7750-014-X. [Google Scholar]
- van Belle, G. Statistical Rules of Thumb, 2nd ed.; Wiley Series in Probability and Statistics; Wiley: Hoboken, NJ, USA, 2011; ISBN 978-1-118-21036-9. [Google Scholar]
- Jian, S.-H.; Yeh, P.-J.; Wang, C.-H.; Chen, H.-C.; Chen, S.-F. Analysis of heterocyclic amines in meat products by liquid chromatography e Tandem mass spectrometry. J. Food Drug Anal. 2019, 27, 595–602. [Google Scholar] [CrossRef] [Green Version]
- Iammarino, M.; Palermo, C.; Nardiello, D.; Muscarella, M. Optimization and Validation of a Confirmatory Method for Determination of Ten Sulfonamides in Feeds by LC and UV-Diode Array Detection. Chromatographia 2011, 73, 75–82. [Google Scholar] [CrossRef]
- McGeehan, S.; Baszler, T.; Gaskill, C.; Johnson, J.; Smith, L.; Raisbeck, M.; Schrier, N.; Harris, H.; Talcott, P. Interlaboratory comparison of heavy metal testing in animal diagnostic specimens and feed using inductively coupled plasma–mass spectrometry. J. Vet. Diagn. Investig. 2020, 32, 291–300. [Google Scholar] [CrossRef] [PubMed]
- Mandel, J. Queries: Regression Analysis of Cumulative Data. Technometrics 1964, 6, 225–227. [Google Scholar] [CrossRef]
- Miller, J.N.; Miller, J.C. Statistics and Chemometrics for Analytical Chemistry, 5th ed.; Pearson Prentice Hall: Harlow, UK; New York, NY, USA, 2005; ISBN 978-0-13-129192-8. [Google Scholar]
- Thompson, M. Recent trends in inter-laboratory precision at ppb and sub-ppb concentrations in relation to fitness for purpose criteria in proficiency testing. Analyst 2000, 125, 385–386. [Google Scholar] [CrossRef]
- Hund, E.; Massart, D.L.; Smeyers-Verbeke, J. Operational De¢nitions of Uncertainty. Trends Anal. Chem. 2001, 20, 14. [Google Scholar] [CrossRef]
- European Commission. Joint Research Centre. The Potential for Expanding Wheat Production and Exports in Kazakhstan: An Analysis from a Food Security Perspective; Publications Office: Luxembourg, 2019. [Google Scholar]
- European Food Safety Authority (EFSA); Medina-Pastor, P.; Triacchini, G. The 2018 European Union report on pesticide residues in food. EFSA J. 2020, 18, e06057. [Google Scholar] [CrossRef] [PubMed] [Green Version]
- European Food Safety Authority (EFSA). National Summary Reports on Pesticide Residue Analysis Performed in 2018. EFSA J. 2020, 17, 1814E. [Google Scholar] [CrossRef]
- Lozowicka, B.; Kaczynski, P.; Paritova, A.А.; Kuzembekova, G.B.; Abzhalieva, A.B.; Sarsembayeva, N.B.; Alihan, K. Pesticide residues in grain from Kazakhstan and potential health risks associated with exposure to detected pesticides. Food Chem. Toxicol. 2014, 64, 238–248. [Google Scholar] [CrossRef]
Pesticide | Class | CAS Number | Molecular Weight | Solubilization Solvent | Precursor Ions | Diagnostic Ions |
---|---|---|---|---|---|---|
Aldrin | organochlorine | 309-00-2 | 364.9 | Toluene | 262.9 | 190.9; 192.9 |
Azinphos-ethyl | organophosphorus | 2642-71-9 | 345.4 | Acetonitrile | 132.0 | 51.0; 77.0 |
cis-Chlordane | organochlorine | 5103-71-9 | 409.8 | Toluene | 271.7; 372.8 | 236.8; 265.9 |
trans--Chlordane | organochlorine | 5103-74-2 | 409.8 | Toluene | 271.7; 372.8 | 236.8; 265.9 |
Chlorfenvinphos | organophosphorus | 470-90-6 | 359.6 | Acetonitrile | 266.9 | 159.0; 203.0 |
Chlorpyrifos | organophosphorus | 2921-88-2 | 350.6 | Acetonitrile | 314.0 | 258.0 |
Chlorpyrifos-methyl | organophosphorus | 5598-13-0 | 322.5 | Acetonitrile | 125.0; 286.0 | 79.0; 93.0 |
Cyfluthrin | pyrethroid | 1820573-27-0 | 434.3 | Toluene | 206.0 | 151.0; 177.0; 179.0 |
Cypermethrin | pyrethroid | 52315-07-8 | 416.3 | Toluene | 181.0 | 127.0; 152.0 |
p,p’ DDD | organochlorine | 72-54-8 | 320.0 | Toluene | 235.0; 237.0 | 165.0 |
p,p’ DDE | organochlorine | 72-55-9 | 318.0 | Toluene | 246.0; 318.0 | 176.0; 248.0 |
p,p’ DDT | organochlorine | 50-29-3 | 354.5 | Toluene | 235.0; 237.0 | 165.0 |
Deltamethrin | pyrethroid | 52918-63-5 | 505.2 | Acetonitrile | 181.1; 252.8 | 152.0; 92.9 |
Diazinon | organophosphorus | 333-41-5 | 304.3 | Acetonitrile | 137.1 | 54.1; 84.1 |
Dieldrin | organochlorine | 60-57-1 | 380.9 | Toluene | 262.8; 277.0 | 227.8; 241.0 |
α-Endosulfan | organochlorine | 959-98-8 | 406.9 | Toluene | 195.0; 240.0 | 160.0; 206.0 |
β-Endosulfan | organochlorine | 33213-65-9 | 406.9 | Toluene | 195.0; 240.9 | 160.0; 206.0 |
Endosulfan sulphate | organochlorine | 1031-07-8 | 422.9 | Toluene | 238.7; 271.8 | 203.9; 234.9 |
Endrin | organochlorine | 72-20-8 | 380.9 | Toluene | 245.0; 262.9 | 173.0; 193.0 |
Fenthion | organophosphorus | 55-38-9 | 278.3 | Acetonitrile | 245.3; 278.0 | 125.0; 109.0; 169.0 |
Fenvalerate | pyrethroid | 51630-58-1 | 419.9 | Acetonitrile | 125.0; 167.0 | 83.3; 125.0 |
α-HCH | organochlorine | 319-84-6 | 290.8 | Toluene | 181.0; 219.0 | 145.0; 183.0 |
β-HCH | organochlorine | 319-85-7 | 290.8 | Toluene | 181.0; 219.0 | 145.0; 183.0 |
γ-HCH | organochlorine | 58-89-9 | 290.8 | Toluene | 180.9; 218.9 | 144.0; 182.9 |
Heptachlor | organochlorine | 76-44-8 | 373.3 | Toluene | 99.8; 272.0 | 65.0; 237.0 |
Heptachlor exo-epoxide | organochlorine | 1024-57-3 | 389.3 | Toluene | 262.9; 352.8 | 192.9; 262.9 |
Heptachlor endo-epoxide | organochlorine | 28044-83-9 | 389.3 | Toluene | 183.0 | 119.0; 155.0 |
Malathion | organophosphorus | 121-75-5 | 330.4 | Acetonitrile | 158.0; 173.1 | 125.0; 99.0 |
Parathion-ethyl | organophosphorus | 56-38-2 | 291.3 | Acetonitrile | 109.0; 291.0 | 81.0; 109.0 |
Permethrin | pyrethroid | 52645-53-1 | 391.3 | Toluene | 183.0 | 128.0; 152.0; 168.0 |
Phenothrin | pyrethroid | 26002-80-2 | 350.4 | Acetonitrile | 183.0 | 115.0; 128.0 |
Profenofos | organophosphorus | 41198-08-7 | 373.6 | Acetonitrile | 296.7; 336.9 | 268.9; 266.9 |
Pyrazophos | organophosphorus | 13457-18-6 | 373.4 | Acetonitrile | 221.0 | 148.7; 193.1 |
Pirimiphos-methyl | organophosphorus | 29232-93-7 | 305.3 | Acetonitrile | 290.1 | 125.0; 233.0 |
Quintozene | organochlorine | 82-68-8 | 295.3 | Toluene | 213.8 | 141.9; 178.9 |
Tecnazene | organochlorine | 117-18-0 | 260.9 | Toluene | 214.8 | 143.6; 178.7 |
Triazophos | organophosphorus | 24017-47-8 | 313.3 | Acetonitrile | 161.0 | 105.7; 134.1 |
Analyte | tR a (min) | LOD | LOQ | LOD | LOQ | Recovery ± SD d | Uncertainty |
---|---|---|---|---|---|---|---|
µg L−1 | µg L−1 | µg kg−1 | µg kg−1 | ||||
Solvent b | Matrix: Wheat c | (%) | (%) | ||||
Aldrin | 14.47 | 0.138 | 0.418 | 0.154 | 0.466 | 74.8 ± 8.6 | 11.5 |
Azinphos-ethyl | 23.26 | 0.080 | 0.243 | 0.086 | 0.259 | 110.3 ± 6.5 | 10.2 |
cis-Chlordane | 16.85 | 0.109 | 0.329 | 0.083 | 0.251 | 70.6 ± 7.7 | 23.1 |
trans-Chlordane | 16.40 | 0.115 | 0.349 | 0.143 | 0.381 | 77 ± 12 | 23.8 |
Chlorfenvinphos | 15.90 | 0.020 | 0.060 | 0.147 | 0.446 | 96.3 ± 6.1 | 15.3 |
Chlorpyrifos | 14.66 | 0.015 | 0.045 | 0.057 | 0.173 | 97.7 ± 8.7 | 16.2 |
Chlorpyrifos-methyl | 13.22 | 0.129 | 0.389 | 0.093 | 0.282 | 91.8 ± 6.0 | 15.5 |
Cyfluthrin | 24.57 | 0.063 | 0.192 | 0.122 | 0.369 | 107 ± 15 | 3.3 |
Cypermethrin | 25.05 | 0.081 | 0.245 | 0.168 | 0.510 | 109 ± 11 | 14.6 |
p,p’ DDD | 18.77 | 0.048 | 0.144 | 0.114 | 0.344 | 78.3 ± 4.8 | 7.4 |
p,p’ DDE | 17.49 | 0.130 | 0.394 | 0.025 | 0.077 | 74.9 ± 5.0 | 13.9 |
p,p’ DDT | 19.87 | 0.186 | 0.565 | 0.101 | 0.306 | 71 ± 10 | 5.9 |
Deltamethrin | 27.25 | 0.152 | 0.460 | 0.018 | 0.056 | 104 ± 14 | 6.7 |
Diazinon | 11.78 | 0.107 | 0.324 | 0.037 | 0.113 | 97 ± 11 | 20.2 |
Dieldrin | 17.54 | 0.148 | 0.450 | 0.035 | 0.106 | 77.2 ± 6.6 | 13.7 |
α-Endosulfan | 16.76 | 0.111 | 0.337 | 0.106 | 0.322 | 79.6 ± 5.3 | 15.5 |
β-Endosulfan | 18.50 | 0.134 | 0.406 | 0.078 | 0.237 | 83.0 ± 5.3 | 9.9 |
Endosulfan sulphate | 19.77 | 0.174 | 0.527 | 0.121 | 0.367 | 92.6 ± 8.1 | 16.8 |
Endrin | 18.20 | 0.170 | 0.515 | 0.160 | 0.484 | 83 ± 14 | 15.4 |
Fenthion | 14.62 | 0.035 | 0.107 | 0.068 | 0.207 | 86 ± 11 | 10.1 |
Fenvalerate | 26.34 | 0.038 | 0.115 | 0.117 | 0.353 | 104 ± 11 | 13.2 |
α-HCH | 10.48 | 0.151 | 0.458 | 0.075 | 0.226 | 81.3 ± 9.7 | 7.8 |
β-HCH | 11.36 | 0.111 | 0.335 | 0.061 | 0.186 | 81.6 ± 9.1 | 10.2 |
γ-HCH | 11.40 | 0.142 | 0.430 | 0.084 | 0.255 | 82 ± 10 | 8.6 |
Heptachlor | 13.44 | 0.119 | 0.361 | 0.095 | 0.288 | 73 ± 12 | 18.8 |
Heptachlor exo-epoxide | 15.67 | 0.140 | 0.424 | 0.148 | 0.449 | 72.5 ± 5.6 | 8.9 |
Heptachlor endo-epoxide | 15.81 | 0.117 | 0.356 | 0.036 | 0.108 | 79.8 ± 9.9 | 11.7 |
Malathion | 14.32 | 0.076 | 0.231 | 0.092 | 0.279 | 108 ± 12 | 13.9 |
Parathion-ethyl | 14.73 | 0.085 | 0.258 | 0.083 | 0.250 | 100.2 ± 9.2 | 12.1 |
Permethrin | 23.85 | 0.050 | 0.152 | 0.091 | 0.273 | 95 ± 11 | 17.7 |
Phenothrin | 22.19 | 0.055 | 0.167 | 0.163 | 0.495 | 91 ± 19 | 22.3 |
Profenofos | 17.38 | 0.129 | 0.391 | 0.098 | 0.296 | 100.9 ± 7.2 | 9.6 |
Pyrazophos | 23.21 | 0.198 | 0.599 | 0.054 | 0.163 | 99.1 ± 6.6 | 9.0 |
Pirimiphos-methyl | 14.06 | 0.031 | 0.094 | 0.138 | 0.418 | 88.9 ± 4.4 | 17.6 |
Quintozene | 11.54 | 0.067 | 0.204 | 0.018 | 0.053 | 87.4 ± 8.1 | 15.4 |
Tecnazene | 9.13 | 0.071 | 0.214 | 0.081 | 0.246 | 76.5 ± 7.3 | 7.6 |
Triazophos | 19.30 | 0.135 | 0.410 | 0.126 | 0.381 | 103.8 ± 6.6 | 11.3 |
Year | Contaminated Matrix | Pesticide | Contamination Level (mg kg−1) | MRL (mg kg−1) |
---|---|---|---|---|
2018 | Wheat | Chlorpyrifos | 0.025 | 0.04 |
Wheat | Fenvalerate | 0.018 | 0.20 | |
Wheat | Cyfluthrin | 0.011 | 0.05 | |
Wheat | Phenothrin | 0.013 | 0.05 | |
Wheat | Deltamethrin | 0.012 | 1.00 | |
Wheat | Deltamethrin | 0.018 | 1.00 | |
Wheat | Cypermethrin | 0.018 | 2.00 | |
Wheat | Cypermethrin | 0.081 | 2.00 | |
Wheat | Pirimiphos-methyl | 0.013 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.030 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.049 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.093 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.113 | 5.00 | |
2019 | Wheat | Pirimiphos-methyl | 0.015 | 5.00 |
Wheat | Pirimiphos-methyl | 0.016 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.018 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.045 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.052 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.054 | 5.00 | |
Wheat | Pirimiphos-methyl | 0.030 | 5.00 | |
Durum wheat bran | Pirimiphos-methyl | 0.080 | 5.00 | |
Oat flakes | Pirimiphos-methyl | 0.020 | 5.00 |
Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affiliations. |
© 2021 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
Share and Cite
Nardelli, V.; D’Amico, V.; Ingegno, M.; Della Rovere, I.; Iammarino, M.; Casamassima, F.; Calitri, A.; Nardiello, D.; Li, D.; Quinto, M. Pesticides Contamination of Cereals and Legumes: Monitoring of Samples Marketed in Italy as a Contribution to Risk Assessment. Appl. Sci. 2021, 11, 7283. https://doi.org/10.3390/app11167283
Nardelli V, D’Amico V, Ingegno M, Della Rovere I, Iammarino M, Casamassima F, Calitri A, Nardiello D, Li D, Quinto M. Pesticides Contamination of Cereals and Legumes: Monitoring of Samples Marketed in Italy as a Contribution to Risk Assessment. Applied Sciences. 2021; 11(16):7283. https://doi.org/10.3390/app11167283
Chicago/Turabian StyleNardelli, Valeria, Valeria D’Amico, Mariateresa Ingegno, Ines Della Rovere, Marco Iammarino, Francesco Casamassima, Anna Calitri, Donatella Nardiello, Donghao Li, and Maurizio Quinto. 2021. "Pesticides Contamination of Cereals and Legumes: Monitoring of Samples Marketed in Italy as a Contribution to Risk Assessment" Applied Sciences 11, no. 16: 7283. https://doi.org/10.3390/app11167283
APA StyleNardelli, V., D’Amico, V., Ingegno, M., Della Rovere, I., Iammarino, M., Casamassima, F., Calitri, A., Nardiello, D., Li, D., & Quinto, M. (2021). Pesticides Contamination of Cereals and Legumes: Monitoring of Samples Marketed in Italy as a Contribution to Risk Assessment. Applied Sciences, 11(16), 7283. https://doi.org/10.3390/app11167283