Simultaneous determination of illegal drug substances in dietary supplements for gout and osteoporosis using ultra-performance liquid chromatography and liquid chromatography-quadrupole-time-of-flight mass spectrometry

Kim, Nam Sook; Kim, Jihee; Lim, Na Young; Lee, Ji Hyun; Park, Seongsoo; Kang, Hoil

doi:10.1016/j.jpba.2019.113003

Cited by 20 publications

(10 citation statements)

References 16 publications

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“…Under the optimized conditions, LODs ranged from 0.1 to 16 ng/g. Furthermore, most substances adulterated in illegal drugs and supplements were found at mg/g levels [41][42][43][44]. Considering the concentration levels of detected adulterants in previous studies, this method enabled sensitive detection for screening of 92 illegal adulterants.…”

Section: Methods Applicationsmentioning

confidence: 89%

Efficient Matrix Cleanup of Soft-Gel-Type Dietary Supplements for Rapid Screening of 92 Illegal Adulterants Using EMR-Lipid dSPE and UHPLC-Q/TOF-MS

et al. 2021

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An efficient matrix cleanup method was developed for the rapid screening of 92 illegal adulterants (25 erectile dysfunction drugs, 15 steroids, seven anabolic steroids, 12 antihistamines, 12 nonsteroidal anti-inflammatory drugs (NSAIDs), four diuretics, and 17 weight-loss drugs) in soft-gel-type supplements by ultra-high performance liquid chromatography-quadrupole/time of flight-mass spectrometry (UHPLC-Q/TOF-MS). As representative green chemistry methods, three sample preparation methods (dispersive liquid-liquid microextraction (DLLME), “quick, easy, cheap, effective, rugged, and safe” dispersive solid-phase extraction (QuEChERS-dSPE), and enhanced matrix removal-lipid (EMR-Lipid) dSPE) were evaluated for matrix removal efficiency, recovery rate, and matrix effect. In this study, EMR-Lipid dSPE was shown to effectively remove complicated matrix contents in soft-gels, compared to DLLME and QuEChERS-dSPE. For the rapid screening of a wide range of adulterants, extracted common ion chromatogram (ECIC) and neutral loss scan (NLS) based on specific common MS/MS fragments were applied to randomly collected soft-gel-type dietary supplement samples using UHPLC-Q/TOF-MS. Both ECICs and NLSs enabled rapid and simple screening of multi-class adulterants and could be an alternative to the multiple reaction monitoring (MRM) method. The developed method was validated in terms of limit of detection (LOD), precision, accuracy, recovery, and matrix effects. The range of LODs was 0.1–16 ng/g. The overall precision values were within 0.09–14.65%. The accuracy ranged from 81.6% to 116.6%. The recoveries and matrix effects of 92 illegal adulterants ranged within 16.9–119.4% and 69.8–114.8%, respectively. The established method was successfully applied to screen and identify 92 illegal adulterants in soft-gels. This method can be a promising tool for the high-throughput screening of various adulterants in dietary supplements and could be used as a more environmentally friendly routine analytical method for screening dietary supplements illegally adulterated with multi-class drug substances.

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Section: Methods Applicationsmentioning

confidence: 89%

Efficient Matrix Cleanup of Soft-Gel-Type Dietary Supplements for Rapid Screening of 92 Illegal Adulterants Using EMR-Lipid dSPE and UHPLC-Q/TOF-MS

et al. 2021

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“…The stability of the 14 drug substances was determined by storing the samples for 24 h and 48 h in an autosampler at 8°C and storing three different concentrations (low, medium, and high) at approximately 8°C for 6 h (n = 3). Matrix effects (%) were also evaluated by comparing two slopes obtained from the calibration curves of the reference standards dissolved in methanol and of standards in spiked blank samples 27 …”

Section: Methodsmentioning

confidence: 99%

“…Finally, the sample solution was filtered using a 0.22 μm polytetrafluoroethylene filter (Millipore, Milford, USA) and then injected into the LC/ESI‐MS/MS apparatus. The sample preparation conditions were based on literature reports 27,28 …”

Section: Methodsmentioning

confidence: 99%

Application of a simultaneous screening method for the detection of new psychoactive substances in various matrix samples using liquid chromatography/electrospray ionization tandem mass spectrometry and liquid chromatography/quadrupole time‐of‐flight mass spectrometry

Kim

Lim

Choi

et al. 2021

Rapid Comm Mass Spectrometry

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Rationale Recently, new psychoactive substances (NPS) have emerged as a public health risk. Particularly, their chemical structures are modified to avoid detection. Synthetic NPS with effects similar to those of illegal drugs have been recently detected and synthesized worldwide, including MDMB‐FUBINACA and APINAC, making it essential to rapidly and accurately detect NPS. Methods Fourteen NPS with similar structures were selected and their structures identified using 1H and 13C NMR spectroscopy. Additionally, we proposed the fragmentation pattern of each compound using liquid chromatography/quadrupole time‐of‐flight mass spectrometry (LC/QTOF‐MS). A simultaneous analytical method using liquid chromatography/electrospray ionization tandem mass spectrometry (LC/ESI‐MS/MS) was also developed and applied to real samples to detect the 14 NPS. The method was validated based on the specificity, linearity, limit of detection (LOD), limit of quantification (LOQ), precision, accuracy, matrix effect, and stability according to international validation guidelines. Results The established method was used to screen 65 different matrix samples using LC/ESI‐MS/MS. By comparing the calculated product ion ratios with those of standards, 2C‐B in one of the real samples and 5F‐MDMB‐PICA in 20 samples were identified. For re‐confirmation of detected compounds, the fragmentation pattern of each compound was compared with that of each standard using LC/QTOF‐MS. Conclusions In this study, LC/QTOF‐MS data were used to elucidate the structures and fragmentation patterns of 14 NPS. A simultaneous method was developed using LC/ESI‐MS/MS, which was applied to 65 real samples. The presented method and results can assist in ensuring the safety of public health from illegal adulteration.

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“…Matrix effects for solid and liquid blank samples were calculated by comparing the slopes of the calibration curves of blank samples spiked with the standards with those obtained for standards dissolved in the solvent 20,21 . The method validation followed the International Council for Harmonization (ICH) guidelines, and all experiments were conducted in triplicate 22–24 …”

Section: Methodsmentioning

confidence: 99%

“…20,21 The method validation followed the International Council for Harmonization (ICH) guidelines, and all experiments were conducted in triplicate. [22][23][24] 2.4 | Preparation conditions and applicability tests Figure 1).…”

Section: Introductionmentioning

confidence: 99%

Simultaneous screening of dietary supplements for 25 anti‐hyperlipidemic substances using ultra‐performance liquid chromatography and liquid chromatography/electrospray ionization tandem mass spectrometry

Kim

Lim

Choi

et al. 2020

Rapid Comm Mass Spectrometry

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RationaleRecently, illegal dietary supplements containing unauthorized compounds have been seized and internationally publicized with a warning to avoid their consumption. This adulteration can be a serious threat to public health because of insufficient and reliable safety data as well as their undesirable side effects. It is, therefore, essential to rapidly and accurately develop and simultaneously validate analytical methods for these unauthorized anti‐hyperlipidemic substances.MethodsDietary supplements were screened simultaneously for 25 anti‐hyperlipidemic drugs using an ultra‐high‐performance liquid chromatography (UPLC) system with a photodiode array (PDA) detector and LC/electrospray ionization tandem mass spectrometry (LC/ESI‐MS/MS). The method validation, according to ICH guidelines, considered specificity, linearity, limit of detection (LOD), limit of quantification (LOQ), precision, accuracy, matrix effects, and stability for solid and liquid blank samples. The established UPLC‐PDA and LC/ESI‐MS/MS methods were applied to screen 103 dietary supplements for 25 anti‐hyperlipidemic substances.ResultsUsing the validated methods, the screened samples were found to contain peaks with similar retention times and PDA spectra. By comparing the calculated precursor‐product ion ratios with those of standards, lovastatin and lovastatin acid were detected at concentrations from LOQ to 4.12 mg/g and LOQ to 9.65 mg/g, respectively.ConclusionsThe developed UPLC‐PDA and LC/ESI‐MS/MS analytical methods were applied to 103 real samples, of which 13 samples were found to contain lovastatin and lovastatin acid. In view of the increasing demand for dietary supplements in the treatment of hyperlipidemic diseases, widespread use of these methods will contribute to consumer health by ensuring the safety of dietary supplements.

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Simultaneous determination of illegal drug substances in dietary supplements for gout and osteoporosis using ultra-performance liquid chromatography and liquid chromatography-quadrupole-time-of-flight mass spectrometry

Cited by 20 publications

References 16 publications

Efficient Matrix Cleanup of Soft-Gel-Type Dietary Supplements for Rapid Screening of 92 Illegal Adulterants Using EMR-Lipid dSPE and UHPLC-Q/TOF-MS

Efficient Matrix Cleanup of Soft-Gel-Type Dietary Supplements for Rapid Screening of 92 Illegal Adulterants Using EMR-Lipid dSPE and UHPLC-Q/TOF-MS

Application of a simultaneous screening method for the detection of new psychoactive substances in various matrix samples using liquid chromatography/electrospray ionization tandem mass spectrometry and liquid chromatography/quadrupole time‐of‐flight mass spectrometry

Simultaneous screening of dietary supplements for 25 anti‐hyperlipidemic substances using ultra‐performance liquid chromatography and liquid chromatography/electrospray ionization tandem mass spectrometry

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