Malaysian Journal of Analytical Sciences, Vol 27 No 1 (2023): 1 - 7

ANALYSIS OF ILLICIT DRUGS IN MUNICIPAL WASTEWATER USING LC-MS/MS: A METHOD VALIDATION STUDY

(Analisa Dadah Berbahaya dalam Air Sisa Perbandaran Menggunakan LC-MS/MS:

Satu Kajian Pengesahan Kaedah)

Mohammad Azimuddin Izani¹, Nurul `Azyyati Sabri¹, Nurul Nadiah Hamidon¹, Kooi Yeong Khaw²,

Iekhsan Othman³, Jochen Mueller⁴ and Joo Hui Tay^1*

¹Faculty of Industrial Sciences & Technology,

Universiti Malaysia Pahang,

Lebuhraya Persiaran Tun Khalil Yaacob, 26300 Gambang, Pahang, Malaysia

² School of Pharmacy, Monash University Malaysia,

Jalan Lagoon Selatan, 47500 Bandar Sunway, Selangor, Malaysia

³Jeffrey Cheah School of Medicine & Health Sciences,

Monash University Malaysia, Jalan Lagoon Selatan, 47500 Bandar Sunway, Selangor, Malaysia

⁴Queensland Alliance for Environmental Health Sciences (QAEHS),

The University of Queensland, 4102, Brisbane, Australia

^*Corresponding author: tayjoohui@ump.edu.my

Received: 19 September 2022; Accepted: 18 December 2022; Published: 22 February 2023

Abstract

An analytical method based on solid-phase extraction (SPE) liquid chromatography-tandem mass spectrometry (LC-MS/MS) for the determination of five illicit drugs, namely amphetamine (AM), methamphetamine (MA), 3,4-methylenedioxymethamphetamine (MDMA), 3,4-methylenedioxyamphetamine (MDA), and morphine (MOR) in municipal wastewater has been optimized and validated. Sample preparation was performed using Oasis MCX SPE cartridges. LC separation was performed using a Zorbax Eclipse Plus C₁₈ RRHD column. The linearity of the calibration curve was between 5 ng/mL and 250 ng/mL, with determination coefficient (R²) greater than 0.99, except for morphine. The mean recoveries of target analytes ranged from 91.6 to 112%, and the method demonstrated good inter-day repeatability (coefficient of variation, CV ranged from 2 to 19%). The limit of detection (LOD) for AM, MA, MDMA, MDA, and MOR was 0.29, 0.37, 0.86, 1.09 and 7.56 ng/mL, respectively. The method was applied to municipal wastewater samples collected from sewage treatment plants in Kuantan, Pahang, in which AM, MA and MDA were detected in all 3 samples.

Keywords: amphetamine, illicit drugs, LC-MS/MS, methamphetamine, municipal wastewater

Abstrak

Kaedah analisis berdasarkan spektrometri jisim kromatografi-tandem cecair (LC-MS/MS) untuk penentuan lima dadah berbahaya, iaitu amphetamine (AM), methamphetamine (MA), 3,4-methylenedioxymethamphetamine (MDMA), 3,4methylenedioxyamphetamine (MDA), dan morfin (MOR) dalam air sisa perbandaran telah dioptimumkan dan disahkan. Penyediaan sampel dilakukan menggunakan kartrij SPE Oasis MCX. Pemisahan LC dilakukan dengan menggunakan turus Zorbax Eclipse Plus C₁₈ RRHD. Kelinearan keluk tentukuran bagi semua analit sasaran berada di antara 5 ng/mL dan 250 ng/mL, kecuali morfin. Putara pemulihan analit sasaran berjulat antara 91.6 hingga 112%, dan kaedah ini menunjukkan kebolehulangan antara hari yang baik (pekali variasi berkisar antara 2 hingga 19%). Had pengesanan (LOD) bagi AM, MA, MDMA, MDA dan MOR adalah 0.29, 0.37, 0.86, 1.09 and 7.56 ng/mL. Kaedah ini digunakan untuk sampel air sisa perbandaran yang dikumpulkan dari loji rawatan kumbahan di Kuantan, Pahang, di mana AM, MA dan MDA telah ditemui dalam ketiga-tiga sampel.

Kata kunci: amphetamine, dadah berbahaya, LC-MS/MS, methamphetamine, air sisa perbandaran

References

1. AADK (2020). Buku Maklumat Dadah 2020. https://www.adk.gov.my/buku-maklumat-dadah-2020/ [Access online 21 August 2022].

2. Subedi, B. and B. Loganathan (2016). Environmental emission of pharmaceuticals from wastewater treatment plants in the U.S.A, in persistent organic chemicals in the environment: status and trends in the Pacific basin countries II temporal trends. American Chemistry Society, Washington, DC: pp. 181-202.

3. Yargeau, V., Taylor, B., Li, H., Rodayan, A. and Metcalfe, C. D. (2014). Analysis of drugs of abuse in wastewater from two Canadian cities. Science of the Total Environment 487: 722-730.

4. Lai, F.Y., O'Brien, J., Bruno, R., Hall, W. Prichard, J., Kirkbride, P., Gartner, C., Thai, P., Carter, S., Lloyd, B., Burns, L. and Mueller, J. (2016). Spatial variations in the consumption of illicit stimulant drugs across Australia: A nationwide application of wastewater-based epidemiology. Science of the Total Environment 568: 810-818.

5. Asicioglu, F., Kuloglu Genc, M., Tekin Bulbul, T., Yayla, M., Simsek, S.Z., Adioren, C. and Mercan, S. (2021). Investigation of temporal illicit drugs, alcohol and tobacco trends in Istanbul city: Wastewater analysis of 14 treatment plants. Water Research 190: 116729.

6. Bannwarth, A., Morelato, M., Benaglia, L., Been, F., Esseiva, P., Delemont, O. and Roux, C. (2019). The use of wastewater analysis in forensic intelligence: drug consumption comparison between Sydney and different European cities. Forensic Sciences Research 4(2): 141-151.

7. Du, P., Liu, X., Zhong, G., Zhou, Z., Thomes, M.W., Lee, C.W., Bong, C.W., Zhang, X., Hao, F., Li, X., Zhang, G. and Thai, P.K. (2020). Monitoring consumption of common illicit drugs in Kuala Lumpur, Malaysia, by Wastewater-Cased Epidemiology. International Journal of Environmental Research and Public Health, 17(3): 889.

8. van Nuijs, A.L., Castiglioni, S., Tarcomnicu, I., Postigo, C., Lopez de Alda, M., Neels, H., Zuccato, E., Barcelo, D. and Covaci, A. (2011). Illicit drug consumption estimations derived from wastewater analysis: a critical review. Science of the Total Environment 409(19): 3564-3577.

9. Chiaia, A.C., C. Banta-Green, and J. Field. (2008). Eliminating solid phase extraction with large-volume injection LC/MS/MS: Analysis of illicit and legal drugs and human urine indicators in US wastewaters. Environmental Science & Technology 42: 8841-8848.

10. Kinyua, J., Covaci, A., Maho, W., McCall, A., Neels, H. and van Nuijs, A.L.N. (2015). Sewage-based epidemiology in monitoring the use of new psychoactive substances: Validation and application of an analytical method using LC-MS/MS. Drug Testing and Analysis 7(9): 812-818.

11. Lai, F.Y., Ort, C., Gartner, C., Carter, S., Prichard, J., Kirkbride, P., Bruno, R., Hall, W., Eaglesham, G. and Mueller, J.F. (2011). Refining the estimation of illicit drug consumptions from wastewater analysis: co-analysis of prescription pharmaceuticals and uncertainty assessment. Water Research, 45(15): 4437-4448.

12. EMEA (2015). Guideline on bioanalytical method validation, in EMEA/CHMP/EWP/192217/2009 Rev. 1 Corr. 2**. Committee for Medicinal Products for Human Use (CHMP), European Medicines Agency (EMEA): London, UK.

13. Khan, U. and Nicell, J.A. (2011). Refined sewer epidemiology mass balances and their application to heroin, cocaine and ecstasy. Environment International 37(7): 1236-1252.

14. Choi, P.M., Tscharke, B.J., O'Brien, J.W., Grant, S.C., Kaserzon, S.L., Mackie, R., O'Malley, E., Crosbie, N.D., Thomas, K.V. and Mueller, J.F. (2018). Wastewater-based epidemiology biomarkers: Past, present and future. Trends in Analytical Chemistry 105: 453-469.