Analysis of commonly prescribed analgesics using in-silico processing of spectroscopic signals: application to surface water and industrial effluents, and comparative study via green and white assessments
Heba T. Elbalkiny A , Mohamed B. El-Zeiny B and Sarah S. Saleh
A *
+ Author Affiliations
- Author Affiliations
A Analytical Chemistry Department, Faculty of Pharmacy, October University for Modern Sciences and Arts (MSA), 11787 6th October, Giza, Egypt.
B Analytical Chemistry Department, Faculty of Pharmacy, Modern University for Technology and Information (MTI), 12582 Al Hadaba Al Wosta, Cairo, Egypt.
Environmental Chemistry 19(7) 446-459 https://doi.org/10.1071/EN22108
Submitted: 13 October 2022 Accepted: 6 December 2022 Published: 10 February 2023
© 2022 The Author(s) (or their employer(s)). Published by CSIRO Publishing.
Environmental context. Pharmaceuticals find their way to wastewater mainly through hospital and industrial effluents, and in turn affect all living organisms. The routine analysis of different water sources is tedious and of high cost. Our work presents a safe, low-cost method for analysing water samples to ensure proper cleanup of water and its suitability for human and animal use.
Rationale. Analgesics are one of the top classes of commonly prescribed drugs, and used over the counter. Therefore, they are most likely to be detected in wastewater samples coming from hospital and industrial effluents.
Methodology. This study focused on developing an in-silico UV spectroscopic manipulation of variant signal nature of low cost, using the methods of: advanced amplitude centring (AAC), mean centring of ratio spectra (MCR), successive derivative subtraction (SDS) and continuous wavelet transformation (CWT), for the determination of a ternary mixture of three analgesics: paracetamol (PCM), diclofenac (DCF) and ibuprofen (IBU) in water samples after sample cleanup using dispersive liquid–liquid microextraction (DLLME).
Results. The proposed methods were compared to those reported in terms of greenness, simplicity and effectiveness using the greenness assessment tools (Eco-scale & AGREE) and white analytical chemistry (WAC) tool. The AAC method showed the highest scores: an Eco-scale of 71, AGREE of 0.55 and RGB of 84.4 when compared to the reported methods.
Discussion. The AAC method was applied effectively for the study of surface water samples and industrial effluents with high accuracy and precision. Thus, real water samples could be routinely analysed with minimal cost to ensure proper cleanup of water and its suitability for human and animal use.
Keywords: AGREE, Diclofenac, dispersive liquid microextraction, Eco-scale, Ibuprofen, Paracetamol, WAC, wavelet.
References
Aguilar-Arteaga K, Rodriguez JA, Miranda JM, Medina J, Barrado E (2010). Determination of non-steroidal anti-inflammatory drugs in wastewaters by magnetic matrix solid phase dispersion–HPLC. Talanta 80, 1152–1157.| Determination of non-steroidal anti-inflammatory drugs in wastewaters by magnetic matrix solid phase dispersion–HPLC.Crossref | GoogleScholarGoogle Scholar |
Al-Kaf AG, Naji KM, Abdullah QYM, Edrees WHA (2017). Occurrence of Paracetamol in Aquatic Environments and Transformation by Microorganisms: A Review. Chronicles of Pharmaceutical Science 1, 341–355.
Andrade-Eiroa A, Canle M, Leroy-Cancellieri V, Cerdà V (2016). Solid-phase extraction of organic compounds: A critical review (Part I). TrAC Trends in Analytical Chemistry 80, 641–654.
| Solid-phase extraction of organic compounds: A critical review (Part I).Crossref | GoogleScholarGoogle Scholar |
Attimarad M, Venugopala KN, Nair AB, Sreeharsha N, Molina EIP, Kotnal RB, Tratrat C, Altaysan AI, Balgoname AA, Deb PK (2022). Environmental sustainable mathematically processed UV spectroscopic methods for quality control analysis of remogliflozin and teneligliptin: Evaluation of greenness and whiteness. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 278, 121303
| Environmental sustainable mathematically processed UV spectroscopic methods for quality control analysis of remogliflozin and teneligliptin: Evaluation of greenness and whiteness.Crossref | GoogleScholarGoogle Scholar |
Avino P, Notardonato I, Passarella S, Russo MV (2020). Determination of non-steroidal anti-inflammatory drugs in animal urine samples by ultrasound vortex-assisted dispersive liquid–liquid microextraction and gas chromatography coupled to ion trap-mass spectrometry. Applied Sciences 10, 5441
| Determination of non-steroidal anti-inflammatory drugs in animal urine samples by ultrasound vortex-assisted dispersive liquid–liquid microextraction and gas chromatography coupled to ion trap-mass spectrometry.Crossref | GoogleScholarGoogle Scholar |
Botrel BMC, Abreu DCP, Saczk AA, Bazana MJF, de Fátima Nascimento C, e Rosa PV (2017). Dispersive liquid-liquid microextraction for the determination of menthol residue in fish by GC–MS. Microchemical Journal, 133, 70–75.
| Dispersive liquid-liquid microextraction for the determination of menthol residue in fish by GC–MS.Crossref | GoogleScholarGoogle Scholar |
Caban M, Mioduszewska K, Łukaszewicz P, Migowska N, Stepnowski P, Kwiatkowski M, Kumirska J (2014). A new silylating reagent – dimethyl(3,3,3-trifluoropropyl)silyldiethylamine – for the derivatisation of non-steroidal anti-inflammatory drugs prior to gas chromatography–mass spectrometry analysis. Journal of Chromatography A 1346, 107–116.
| A new silylating reagent – dimethyl(3,3,3-trifluoropropyl)silyldiethylamine – for the derivatisation of non-steroidal anti-inflammatory drugs prior to gas chromatography–mass spectrometry analysis.Crossref | GoogleScholarGoogle Scholar |
Diuzheva A, Balogh J, Jekő J, Cziáky Z (2018). Application of liquid–liquid microextraction for the effective separation and simultaneous determination of 11 pharmaceuticals in wastewater samples using high‐performance liquid chromatography with tandem mass spectrometry. Journal of Separation Science 41, 2870–2877.
| Application of liquid–liquid microextraction for the effective separation and simultaneous determination of 11 pharmaceuticals in wastewater samples using high‐performance liquid chromatography with tandem mass spectrometry.Crossref | GoogleScholarGoogle Scholar |
Duncan D, Harvey F, Walker M, Australian Water Quality Centre (2007) ‘EPA guide line: Regulatory monitoring and testing Water and wastewater sampling.’ (Environment Protection Authority: South Australia)
El-Hanboushy S, Marzouk HM, Fayez YM, Abdelkawy M, Lotfy HM (2022). Sustainable spectrophotometric determination of antihypertensive medicines reducing COVID-19 risk via paired wavelength data processing technique - Assessment of purity, greenness and whiteness. Sustainable Chemistry and Pharmacy 29, 100806
| Sustainable spectrophotometric determination of antihypertensive medicines reducing COVID-19 risk via paired wavelength data processing technique - Assessment of purity, greenness and whiteness.Crossref | GoogleScholarGoogle Scholar |
El-Shorbagy HI, Belal F (2022). Innovative derivative/zero ratio spectrophotometric method for simultaneous determination of sofosbuvir and ledipasvir: Application to average content and uniformity of dosage units. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 267, 120623
| Innovative derivative/zero ratio spectrophotometric method for simultaneous determination of sofosbuvir and ledipasvir: Application to average content and uniformity of dosage units.Crossref | GoogleScholarGoogle Scholar |
Gałuszka A, Migaszewski Z, Namieśnik J (2013). The 12 principles of green analytical chemistry and the SIGNIFICANCE mnemonic of green analytical practices. TrAC Trends in Analytical Chemistry 50, 78–84.
| The 12 principles of green analytical chemistry and the SIGNIFICANCE mnemonic of green analytical practices.Crossref | GoogleScholarGoogle Scholar |
Hennion M-C (1999). Solid-phase extraction: method development, sorbents, and coupling with liquid chromatography. Journal of Chromatography A 856, 3–54.
| Solid-phase extraction: method development, sorbents, and coupling with liquid chromatography.Crossref | GoogleScholarGoogle Scholar |
Jaleh B, Fakhri P (2016) Chapter 5 - Infrared and Fourier transform infrared spectroscopy for nanofillers and their nanocomposites. In ‘Spectroscopy of Polymer Nanocomposites’. (Eds S Thomas, D Rouxel, D Ponnamma) (William Andrew Publishing)
Kelani KM, Elzanfaly ES, Saad AS, Halim MK, El-Zeiny MB (2021). Different greenness assessment perspectives for stability-indicating RP-HPLC method used for the assay of isoxsuprine hydrochloride and four nephrotoxic and hepatotoxic photothermal degradation products. Microchemical Journal 171, 106826
| Different greenness assessment perspectives for stability-indicating RP-HPLC method used for the assay of isoxsuprine hydrochloride and four nephrotoxic and hepatotoxic photothermal degradation products.Crossref | GoogleScholarGoogle Scholar |
Kümmerer K (2008) ‘Pharmaceuticals in the environment: sources, fate, effects and risks.’ (Springer Science & Business Media)
Larsson DGJ, de Pedro C, Paxeus N (2007). Effluent from drug manufactures contains extremely high levels of pharmaceuticals. Journal of Hazardous Materials 148, 751–755.
| Effluent from drug manufactures contains extremely high levels of pharmaceuticals.Crossref | GoogleScholarGoogle Scholar |
Li J, Ye Q, Gan J (2014). Degradation and transformation products of acetaminophen in soil. Water Research 49, 44–52.
| Degradation and transformation products of acetaminophen in soil.Crossref | GoogleScholarGoogle Scholar |
Liška I (2000). Fifty years of solid-phase extraction in water analysis – historical development and overview. Journal of Chromatography A 885, 3–16.
| Fifty years of solid-phase extraction in water analysis – historical development and overview.Crossref | GoogleScholarGoogle Scholar |
Liu H, Dasgupta PK (1996). Analytical chemistry in a drop. Solvent extraction in a microdrop. Analytical Chemistry, 68, 1817–1821.
| Analytical chemistry in a drop. Solvent extraction in a microdrop.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Saleh SS (2018). Testing the purity of spectral profiles: finger-print resolution of complex matrices and extraction of absorbance signals. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 205, 160–169.
| Testing the purity of spectral profiles: finger-print resolution of complex matrices and extraction of absorbance signals.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Saleh SS (2019). Investigating Advanced Approaches Based on Iso-Absorptivity Coefficient in Unresolved Spectral Signals of Binary Mixtures. Journal of Analytical Methods in Chemistry 2019, 7924821
| Investigating Advanced Approaches Based on Iso-Absorptivity Coefficient in Unresolved Spectral Signals of Binary Mixtures.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Hassan NY, Elgizawy SM, Saleh SS (2013). Comparative Study of New Spectrophotometric Methods; an Application on Pharmaceutical Binary Mixture of Ciprofloxacin Hydrochloride and Hydrocortisone. Journal of the Chilean Chemical Society 58, 1892–1898.
| Comparative Study of New Spectrophotometric Methods; an Application on Pharmaceutical Binary Mixture of Ciprofloxacin Hydrochloride and Hydrocortisone.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Tawakkol SM, Fahmy NM, Shehata MA (2014). Successive spectrophotometric resolution as a novel technique for the analysis of ternary mixtures of pharmaceuticals. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 121, 313–323.
| Successive spectrophotometric resolution as a novel technique for the analysis of ternary mixtures of pharmaceuticals.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Saleh SS, Hassan NY, Salem H (2015). Computation of geometric representation of novel spectrophotometric methods used for the analysis of minor components in pharmaceutical preparations. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 151, 628–643.
| Computation of geometric representation of novel spectrophotometric methods used for the analysis of minor components in pharmaceutical preparations.Crossref | GoogleScholarGoogle Scholar |
Lotfy HM, Saleh SS, El-Maraghy CM (2020). Advanced approaches for the treatment and amplification of weak spectral signals produced by critical concentrations in white multicomponent systems. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 224, 117339
| Advanced approaches for the treatment and amplification of weak spectral signals produced by critical concentrations in white multicomponent systems.Crossref | GoogleScholarGoogle Scholar |
Mowaka S, Hegazy MA, Lotfy HM, Mohamed EH (2017). Novel pure component contribution algorithm (PCCA) and UHPLC methods for separation and quantification of amlodipine, valsartan, and hydrochlorothiazide in ternary mixture. Journal of AOAC International 100, 692–699.
| Novel pure component contribution algorithm (PCCA) and UHPLC methods for separation and quantification of amlodipine, valsartan, and hydrochlorothiazide in ternary mixture.Crossref | GoogleScholarGoogle Scholar |
Nowak PM, Wietecha-Posłuszny R, Pawliszyn J (2021). White Analytical Chemistry: An approach to reconcile the principles of Green Analytical Chemistry and functionality. TrAC Trends in Analytical Chemistry 138, 116223
| White Analytical Chemistry: An approach to reconcile the principles of Green Analytical Chemistry and functionality.Crossref | GoogleScholarGoogle Scholar |
Pena-Pereira F, Wojnowski W, Tobiszewski M (2020). AGREE—Analytical GREEnness metric approach and software. Analytical Chemistry 92, 10076–10082.
| AGREE—Analytical GREEnness metric approach and software.Crossref | GoogleScholarGoogle Scholar |
Pharmacopoeia B (2009) The Stationery Office on behalf of the Medicines and Healthcare products Regulatory Agency (MHRA)-© Crown Copyright.
Qiting J, Xiheng Z (1988). Combination process of anaerobic digestion and ozonization technology for treating wastewater from antibiotics production. Water Treat 3, 285–291.
Rezaee M, Assadi Y, Milani Hosseini M-R, Aghaee E, Ahmadi F, Berijani S (2006). Determination of organic compounds in water using dispersive liquid–liquid microextraction. Journal of Chromatography A, 1116, 1–9.
| Determination of organic compounds in water using dispersive liquid–liquid microextraction.Crossref | GoogleScholarGoogle Scholar |
Riad SM, Salem H, Elbalkiny HT, Khattab FI (2015). Validated univariate and multivariate spectrophotometric methods for the determination of pharmaceuticals mixture in complex wastewater. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 140, 451–461.
| Validated univariate and multivariate spectrophotometric methods for the determination of pharmaceuticals mixture in complex wastewater.Crossref | GoogleScholarGoogle Scholar |
Runnalls TJ, Margiotta-Casaluci L, Kugathas S, Sumpter JP (2010). Pharmaceuticals in the aquatic environment: steroids and anti-steroids as high priorities for research. Human and Ecological Risk Assessment: An International Journal 16, 1318–1338.
| Pharmaceuticals in the aquatic environment: steroids and anti-steroids as high priorities for research.Crossref | GoogleScholarGoogle Scholar |
Sajid M, Płotka-Wasylka J (2022). Green analytical chemistry metrics: A review. Talanta 238, 123046
| Green analytical chemistry metrics: A review.Crossref | GoogleScholarGoogle Scholar |
Saleh SS, Lotfy HM, Hassan NY, Salem H (2014). A comparative study of progressive versus successive spectrophotometric resolution techniques applied for pharmaceutical ternary mixtures. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 132, 239–248.
| A comparative study of progressive versus successive spectrophotometric resolution techniques applied for pharmaceutical ternary mixtures.Crossref | GoogleScholarGoogle Scholar |
Saleh SS, Lotfy HM, Tiris G, Erk N, Rostom Y (2020). Analytical tools for greenness assessment of chromatographic approaches: Application to pharmaceutical combinations of Indapamide, Perindopril and Amlodipine. Microchemical Journal 159, 105557
| Analytical tools for greenness assessment of chromatographic approaches: Application to pharmaceutical combinations of Indapamide, Perindopril and Amlodipine.Crossref | GoogleScholarGoogle Scholar |
Salem H, Lotfy HM, Hassan NY, El-Zeiny MB, Saleh SS (2015). A comparative study of different aspects of manipulating ratio spectra applied for ternary mixtures: Derivative spectrophotometry versus wavelet transform. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 135, 1002–1010.
| A comparative study of different aspects of manipulating ratio spectra applied for ternary mixtures: Derivative spectrophotometry versus wavelet transform.Crossref | GoogleScholarGoogle Scholar |
Santos JL, Aparicio I, Alonso E, Callejón M (2005). Simultaneous determination of pharmaceutically active compounds in wastewater samples by solid phase extraction and high-performance liquid chromatography with diode array and fluorescence detectors. Analytica Chimica Acta 550, 116–122.
| Simultaneous determination of pharmaceutically active compounds in wastewater samples by solid phase extraction and high-performance liquid chromatography with diode array and fluorescence detectors.Crossref | GoogleScholarGoogle Scholar |
Stratil P, Klejdus B, Kubáň V (2006). Determination of total content of phenolic compounds and their antioxidant activity in vegetables evaluation of spectrophotometric methods. Journal of agricultural and food chemistry 54, 607–616.
| Determination of total content of phenolic compounds and their antioxidant activity in vegetables evaluation of spectrophotometric methods.Crossref | GoogleScholarGoogle Scholar |
Turak F, Ozgur MU (2013). Simultaneous determination of allura red and ponceau 4R in drinks with the use of four derivative spectrophotometric methods and comparison with high-performance liquid chromatography. Journal of AOAC International 96, 1377–1386.
| Simultaneous determination of allura red and ponceau 4R in drinks with the use of four derivative spectrophotometric methods and comparison with high-performance liquid chromatography.Crossref | GoogleScholarGoogle Scholar |
Van Aken K, Strekowski L, Patiny L (2006). EcoScale, a semi-quantitative tool to select an organic preparation based on economical and ecological parameters. Beilstein Journal of Organic Chemistry 2, 3
| EcoScale, a semi-quantitative tool to select an organic preparation based on economical and ecological parameters.Crossref | GoogleScholarGoogle Scholar |
Vane JR, Botting RM (1998). Anti-inflammatory drugs and their mechanism of action. Inflammation Research 47, 78–87.
| Anti-inflammatory drugs and their mechanism of action.Crossref | GoogleScholarGoogle Scholar |
Viñas P, Campillo N, López-García I, Hernández-Córdoba M (2014). Dispersive liquid–liquid microextraction in food analysis. A critical review. Analytical and Bioanalytical Chemistry 406, 2067–2099.
| Dispersive liquid–liquid microextraction in food analysis. A critical review.Crossref | GoogleScholarGoogle Scholar |
Weigel S, Kallenborn R, Hühnerfuss H (2004). Simultaneous solid-phase extraction of acidic, neutral and basic pharmaceuticals from aqueous samples at ambient (neutral) pH and their determination by gas chromatography–mass spectrometry. Journal of Chromatography A 1023, 183–195.
| Simultaneous solid-phase extraction of acidic, neutral and basic pharmaceuticals from aqueous samples at ambient (neutral) pH and their determination by gas chromatography–mass spectrometry.Crossref | GoogleScholarGoogle Scholar |
Yehia AM, Elbalkiny HT, Riad SM, Elsaharty YS (2020). Application of Chemometrics for Spectral Resolving and Determination of Three Analgesics in Water Samples. Journal of AOAC International 103, 257–264.
| Application of Chemometrics for Spectral Resolving and Determination of Three Analgesics in Water Samples.Crossref | GoogleScholarGoogle Scholar |
