Validated Chromatography Method for Analysis of Formaldehyde Migration Levels in Bottled Drinking Water
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Keywords:
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Bottled Drinking Water, Formaldehyde, Polyethylene Terephthalate, Validation
Abstract
Polyethylene terephthalate (PET) is utilized in the containment of potable water, nonetheless, it is susceptible to impairment due to temperature and duration of storage. Migration of formaldehyde from PET arises as a consequence of thermal deterioration. This study aims to ascertain the extent of formaldehyde transference in PET-contained drinking water of varying condition, subjected to diverse temperature setting and storage durations. An examination into the levels of formaldehyde migration in polyethylene terephthalate (PET) bottled drinking water was effectively carried out employing a validated high-performance liquid chromatography (HPLC) technique. A total of 162 water samples from three different PET bottled water brands sourced from supermarkets in Palu City, Central Sulawesi, Indonesia, underwent analysis. The formaldehyde assessment was executed utilizing a mobile phase composition of methanol:acetonitrile:water (48:12:40 v/v) for 12.97 minutes at a flow rate of 0.8 mL/minute on the 1st day, the 14th day, and the 42nd day while stored at room temperature and exposed to sunlight. Formaldehyde, lacking effective chromophoric entities and not readily ionizable, necessitated derivatization with 2,4-dinitrophenylhydrazine before HPLC analysis. The findings of the study demonstrated exceptional method linearity within the concentration span of 0.5 to 1321 µg/mL, exhibiting a commendable correlation coefficient of 0.999. The limit of detection (LOD) and quantification (LOQ) were determined to be 17.33 and 57.76 µg/mL, correspondingly. Precision evaluations displayed average intraday and interday values of 128.46±3.48% and 103.19±0.12%, respectively (%RSD < 2/3 CV Horwitz ratio). The intraday and interday %recovery values were computed at 97.22±3.48% and 96.83±0.14% (n = 6). The scrutiny of formaldehyde concentrations in the water samples unveiled the absence of formaldehyde migration.
References
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Islam, M. A., B. G. Jeong, W. L. Kerr, and J. Chun (2021). Validation of Phytosterol Analysis by Alkaline Hydrolysis and Trimethylsilyl Derivatization Coupled with Gas Chromatography For Rice Products. Journal of Cereal Science, 101; 103305
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Latimer Jr, G. (2016). Guidelines for Standard Method Performance Requirements: Official Methods of Analysis. AOAC International; 1–18
López-Fernández, O., R. Domínguez, M. Pateiro, P. E. Munekata, G. Rocchetti, and J. M. Lorenzo (2020). Determination of Polyphenols Using Liquid Chromatography– Tandem Mass Spectrometry Technique (lC–MS/MS): A Review. Antioxidants, 9(6); 479
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Marcela, M. C. I., J. Pereira Dos Anjos, F. Oliveira Campos Da Rocha, and J. B. De andrade (2021). Exploratory Analysis of the Presence of 14 Carbonyl Compounds in Bottled Mineral Water in Polyethylene Terephthalate (Pet) Containers. Food Chemistry, 365; 130475
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Ravisankar, P., C. Naga Navya, D. Pravallika, and D. N. Sri (2015). A Review on Step-by-Step Analytical Method Validation. IOSR Journal of Pharmacy, 5(10); 2250–3013
Rohyami, Y. and R. M. Pribadi (2017). Validation of Methods on Formalin Testing in Tofu and Determination of 3,5- Diacetyl-Dihydrolutidine Stability by UV-Vis Spectrophotometry. In AIP Conference Proceedings, volume 1911
Satwekar, A., A. Panda, P. Nandula, S. Sripada, R. Govindaraj, and M. Rossi (2023). Digital by Design Approach To Develop A Universal Deep Learning AI Architecture For Automatic Chromatographic Peak integration. Biotechnology and Bioengineering, 120(7); 1822–1843
Sebaei, A. S., A. M. Gomaa, A. El-Zwahry, E. Emara, et al. (2018). Determination of Formaldehyde by HPLC with Stable Precolumn Derivatization in Egyptian Dairy Products. International Journal of Analytical Chemistry, 2018; 1–5
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Yoshikawa, K., Y. Oshima, A. inagaki, and A. Sakuragawa (2018). Determination of Formaldehyde in Water Samples by High-Performance Liquid Chromatography with Methyl Acetoacetate Derivatization. Bulletin of Environmental Contamination and Toxicology, 101(5); 672–677
Abdu Hussen, A. (2022). High-Performance Liquid Chromatography (HPLC): A Review. Annals of Advances in Chemistry, 6(1); 010–020
Abe, Y., N. Kobayashi, M. Yamaguchi, M. Mutsuga, A. Ozaki, E. Kishi, and K. Sato (2021). Determination of Formaldehyde and Acetaldehyde Levels in Poly(Ethylene Terephthalate) (Pet) Bottled Mineral Water Using A Simple and Rapid Analytical Method. Food Chemistry, 344; 128708
Alamri, M. S., A. A. A. Qasem, A. A. Mohamed, S. Hussain, M. A. Ibraheem, G. Shamlan, H. A. Alqah, and A. S. Qasha (2021). Food Packaging’s Materials: A Food Safety Perspective. Saudi Journal of Biological Sciences, 28(8); 4490–4499
Ambadekar, S., D. Baburao Nikam, and S. Raju Ambadekar (2020). Formaldehyde in Baby Foods by HPLC-ELSD. American Journal of Chemistry, 2020(2); 19–25
Article, O. R., Y. Vidushi, and B. Meenakshi (2017). A Review on HPLC Method Development and Validation. Unnamed Journal, 2(166); 166–178
Bose, A. (2014). HPLC Calibration Process Parameters in Terms of System Suitability Test. Austin Chromatography, 1(2); 1–4. Available from: www.austinpublishinggroup.com
Chan, C. C., H. Lam, Y. C. Lee, and N. Pharma (2004). Analytical Method Validation and instrument Performance Verification
Cincotta, F., A. Verzera, G. Tripodi, and C. Condurso (2018). Non intentionally Added Substances in Pet Bottled Mineral Water During the Shelf Life. European Food Research and Technology, 244(3); 433–439
Dehghani, M. H., M. Farhang, and A. Zarei (2018). Investigation of Carbonyl Compounds (Acetaldehyde and Formaldehyde) in Bottled Waters in Iranian Markets. International Food Research Journal, 25(2); 876–879
European Commission (2011). Commission Regulation (EU) No 10/2011 of 14 January 2011 on Plastic Materials and Articles Intended to Come into Contact with Food. Official Journal of the European Union, 12; 1–89
Fappiano, L., F. Carriera, A. Iannone, I. Notardonato, and P. Avino (2022). A Review on Recent Sensing Methods For Determining Formaldehyde in Agri-Food Chain: A Comparison with the Conventional Analytical Approaches. Foods, 11(9)
Faria, I. D. L., M. M. Gouvêa, A. D. Pereira Netto, and F. F. de Carvalho Marques (2022). Determination of Formaldehyde in Bovine Milk by Micellar Electrokinetic Chromatography with Diode Array Detection. Lwt, 163
Georgopoulou, M. P. and C. V. Chrysikopoulos (2018). Evaluation of Carbon Nanotubes and Quartz Sand For the Removal of Formaldehyde- (2,4-Dinitrophenylhydrazine) From Aqueous Solutions. Industrial & Engineering Chemistry Research
Gerassimidou, S., P. Lanska, J. N. Hahladakis, E. Lovat, S. Vanzetto, B. Geueke, K. J. Groh, J. Muncke, M. Maffini, O. V. Martin, and E. Iacovidou (2022). Unpacking the Complexity of the Pet Drink Bottles Value Chain: A Chemicals Perspective. Journal of Hazardous Materials, 430; 128410
Gnanavelu, A., T. S. Shanmuganathan, V. Deepesh, and S. Suresh (2021). Validation of A Modified Procedure For the Determination of Chemical Oxygen Demand Using Standard Dichromate Method in Industrial Wastewater Samples with High Calcium Chloride Content
Hanin, N. and D. P. Lestari (2023). Determination of Nitrite in the Kapuas Besar River by Spectrophotometric Method. In Proceeding International Conference on Religion, Sciences, and Education, volume 2. pages 795–800
Haque, M. A., V. Bakshi, M. Thippani, R. M. Manda, and N. Boggula (2021). Development and Validation of UV Spectrophotometric Method For the Determination of Dolutegravir by Using Quality by Design (Qbd) Approach. Journal of Advanced Scientific Research, 12(3). Available from: http://www.sciensage.info
Hossain, M. S., M. S. Islam, S. Bhadra, and A. S. Shamsur Rouf (2016). Investigation of Formaldehyde Content in Dairy Products Available in Bangladesh by A Validated High Performance Liquid Chromatographic Method. Dhaka University Journal of Pharmaceutical Sciences, 15(2); 187–194
Ikhsan, A. N., M. C. Thohira, and D. Daniel (2022). Analysis of Packaged Drinking Water Use in Indonesia in the Last Decades: Trends, Socio-Economic Determinants, and Safety Aspect. Water Policy, 24(8); 1287–1305
Islam, M. A., B. G. Jeong, W. L. Kerr, and J. Chun (2021). Validation of Phytosterol Analysis by Alkaline Hydrolysis and Trimethylsilyl Derivatization Coupled with Gas Chromatography For Rice Products. Journal of Cereal Science, 101; 103305
Jin, X. C., R. M. Ballentine, W. P. Gardner, M. S. Melvin, Y. B. Pithawalla, K. A. Wagner, K. C. Avery, and M. Sharifi (2021). Determination of Formaldehyde Yields in E-Cigarette Aerosols: An Evaluation of the Efficiency of the DNPH Derivatization Method. Separations, 8(9); 151
Latimer Jr, G. (2016). Guidelines for Standard Method Performance Requirements: Official Methods of Analysis. AOAC International; 1–18
López-Fernández, O., R. Domínguez, M. Pateiro, P. E. Munekata, G. Rocchetti, and J. M. Lorenzo (2020). Determination of Polyphenols Using Liquid Chromatography– Tandem Mass Spectrometry Technique (lC–MS/MS): A Review. Antioxidants, 9(6); 479
Lugwisha, E., J. A. Mahugija, and C. Mwankuna (2016). Levels of Formaldehyde and Acetaldehyde in Selected Bottled Drinking Water Sold in Urban Areas in Tanzania. Tanzania Journal of Science, 42(1); 1–14
Marcela, M. C. I., J. Pereira Dos Anjos, F. Oliveira Campos Da Rocha, and J. B. De andrade (2021). Exploratory Analysis of the Presence of 14 Carbonyl Compounds in Bottled Mineral Water in Polyethylene Terephthalate (Pet) Containers. Food Chemistry, 365; 130475
Minister of Industry of the Republic of Indonesia (2016). Mandatory Implementation of the Indonesian National Standard for Mineral Water, Demineralized Water, Natural Mineral Water, and Dewatered Drinking Water. Indonesia
Moldoveanu, S. C. and V. David (2022). Essentials in Modern HPLC Separations Second Edition. Elsevier, Netherlands International Conference on Harmonisation of Technical Requirements For Registratation of Pharmaceuticals For Human Use (2005). Validation of Analytical Procedures: Text and Methodology Q2(R1). November 1996
Protano, C., G. Buomprisco, V. Cammalleri, R. N. Pocino, D. Marotta, S. Simonazzi, F. Cardoni, M. Petyx, S. Iavicoli, and M. Vitali (2022). the Carcinogenic Effects of Formaldehyde Occupational Exposure: A Systematic Review. Cancers, 14(1)
Ravisankar, P., C. Naga Navya, D. Pravallika, and D. N. Sri (2015). A Review on Step-by-Step Analytical Method Validation. IOSR Journal of Pharmacy, 5(10); 2250–3013
Rohyami, Y. and R. M. Pribadi (2017). Validation of Methods on Formalin Testing in Tofu and Determination of 3,5- Diacetyl-Dihydrolutidine Stability by UV-Vis Spectrophotometry. In AIP Conference Proceedings, volume 1911
Satwekar, A., A. Panda, P. Nandula, S. Sripada, R. Govindaraj, and M. Rossi (2023). Digital by Design Approach To Develop A Universal Deep Learning AI Architecture For Automatic Chromatographic Peak integration. Biotechnology and Bioengineering, 120(7); 1822–1843
Sebaei, A. S., A. M. Gomaa, A. El-Zwahry, E. Emara, et al. (2018). Determination of Formaldehyde by HPLC with Stable Precolumn Derivatization in Egyptian Dairy Products. International Journal of Analytical Chemistry, 2018; 1–5
Setyaningsih, D., Y. A. Santoso, Y. S. Hartini, Y. B. Murti, W. L. J. Hinrichs, and C. Patramurti (2021). Isocratic High-Performance Liquid Chromatography (HPLC) For Simultaneous Quantification of Curcumin and Piperine in A Microparticle Formulation Containing Curcuma Longa and Piper Nigrum. Heliyon, 7(3); e06541
Singh, S., N. Sharma, N. Kanojia, G. Kaur, and S. Arora (2020). Development and Validation of UV Spectrophotometer Method for Analysis of Fluvastatin Sodium in PolyethyleneGlycol 6000 and Polyvinyl Pyrollidone K30 Solid Dispersions. Plant Archives, 20(1); 3365–3371
Sulistyaningrum, I., M. P. G. Utami, R. B. Istiningrum, and I. M. Siregar (2015). Comparison Between the Calibration and the Standard Addition Methods in Determining Dissolved Lead in Borobudur’s Control Tanks Water by Flame Atomic Absorption Spectrophotometry (F-AAS). Procedia Chemistry, 17; 70–74
Tsaridou, C. and A. J. Karabelas (2021). Drinking Water Standards and Their Implementation—A Critical Assessment. Water, 13(20); 2918
U.S. Environmental Protection Agency (1992). Method 554. Determination of Carbonyl Compounds in Drinking Water by Dinitrophenylhydrazine Derivatization and High Performance Liquid Chromatography, Rev. 1.0. Methods For the Determination of Organic Compounds in Drinking Water, Suppl. II. U.S. Environmental Protection Agency, Cincinnati, OH
World Health Organization (2005). Mercury in Drinking Water, Background Document For Development of WHO Guidelines For Drinking-Water Quality
Yoshikawa, K., Y. Oshima, A. inagaki, and A. Sakuragawa (2018). Determination of Formaldehyde in Water Samples by High-Performance Liquid Chromatography with Methyl Acetoacetate Derivatization. Bulletin of Environmental Contamination and Toxicology, 101(5); 672–677
Authors
Ramadhani, N., Yulianty, R., Rifai, Y., Aswad, M., Alam, G., Naid, T., & Kasim, A. K. (2024). Validated Chromatography Method for Analysis of Formaldehyde Migration Levels in Bottled Drinking Water. Science and Technology Indonesia, 9(3), 660–668. https://doi.org/10.26554/sti.2024.9.3.660-668
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