A novel quantification method for sulfur-containing biomarkers of formaldehyde and acetaldehyde exposure in human urine and plasma samples

Landmesser, Anne; Scherer, Gerhard; Pluym, Nikola; Scherer, Max

doi:10.1007/s00216-020-02888-y

Cited by 8 publications

(10 citation statements)

References 46 publications

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“…43 Recently, Landmesser et al used 13 C-PG and 13 C-VG to detect sulfur-containing thiazolidine carboxylic acid and thiazolidine carbonyl glycine metabolites of formaldehyde in urine following inhalation exposure to cigarette smoke or to e-cig aerosols, indicating a potential biomarker of form-aldehyde exposure, while a similar biomarker of acetaldehyde inhalation exposure is still needed. 20,40 5. CONCLUSIONS Our data provide further evidence for the formation of toxic compounds (glycidol and acrolein) in e-cigarette aerosols and support a hypothesis that the glycidol metabolite 23HPMA may be useful as a relatively specific biomarker of e-cigarette use.…”

Section: Discussionmentioning

confidence: 99%

Electronic Cigarette Solvents, JUUL E-Liquids, and Biomarkers of Exposure: In Vivo Evidence for Acrolein and Glycidol in E-Cig-Derived Aerosols

Lorkiewicz

Keith

Lynch

et al. 2022

Chem. Res. Toxicol.

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Despite the increasing popularity of e-cigarettes, their long-term health effects remain unknown. In animal models, exposure to e-cigarette has been reported to result in pulmonary and cardiovascular injury, and in humans, the acute use of e-cigarettes increases heart rate and blood pressure and induces endothelial dysfunction. In both animal models and humans, cardiovascular dysfunction associated with e-cigarettes has been linked to reactive aldehydes such as formaldehyde and acrolein generated in e-cigarette aerosols. These aldehydes are known products of heating and degradation of vegetable glycerin (VG) present in e-liquids. Here, we report that in mice, acute exposure to a mixture of propylene glycol:vegetable glycerin (PG:VG) or to e-cigarette-derived aerosols significantly increased the urinary excretion of acrolein and glycidol metabolites—3-hydroxypropylmercapturic acid (3HPMA) and 2,3-dihydroxypropylmercapturic acid (23HPMA)—as measured by UPLC-MS/MS. In humans, the use of e-cigarettes led to an increase in the urinary levels of 23HPMA but not 3HPMA. Acute exposure of mice to aerosols derived from PG: 13 C 3 -VG significantly increased the 13 C 3 enrichment of both urinary metabolites 13 C 3 -3HPMA and 13 C 3 -23HPMA. Our stable isotope tracing experiments provide further evidence that thermal decomposition of vegetable glycerin in the e-cigarette solvent leads to generation of acrolein and glycidol. This suggests that the adverse health effects of e-cigarettes may be attributable in part to these reactive compounds formed through the process of aerosolizing nicotine. Our findings also support the notion that 23HPMA, but not 3HPMA, may be a relatively specific biomarker of e-cigarette use.

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Section: Discussionmentioning

confidence: 99%

Electronic Cigarette Solvents, JUUL E-Liquids, and Biomarkers of Exposure: In Vivo Evidence for Acrolein and Glycidol in E-Cig-Derived Aerosols

Lorkiewicz

Keith

Lynch

et al. 2022

Chem. Res. Toxicol.

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“…Given the observed concentration-dependent formation of PGF and SPro-Gly in both in vitro (Figure B) and cultured HeLa cells (Figure B), the current results shed light on the potential to use these two conjugates as biomarker molecules in connection with formaldehyde and oxidative stress exposure. Furthermore, in contrast to DNA adducts, protein adducts, and DNA–protein cross-link products that were previously used as biomarkers of formaldehyde exposure, − Spro-Gly could be easily detected as it is a urinary metabolite . The detection of urinary SPro-Gly and PGF may serve as a noninvasive tool to carry out an assessment of short-term formaldehyde exposure risk.…”

Section: Resultsmentioning

confidence: 99%

LC-MS/MS Quantitation of Formaldehyde–Glutathione Conjugates as Biomarkers of Formaldehyde Exposure and Exposure-Induced Antioxidants: A New Look on an Old Topic

Ham

Pan

Chan

et al. 2022

Chem. Res. Toxicol.

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Humans are continuously exposed to formaldehyde via both endogenous and exogenous sources. Prolonged exposure to formaldehyde is associated with many human diseases, such as lung cancer and leukemia. The goal of this study is to develop biomarkers to measure formaldehyde exposure, which could be used to predict the risk of associated diseases. As glutathione (GSH) is well-known for its crucial role in the detoxification of a wide variety of xenobiotics, including formaldehyde, we rigorously quantitated in this study the conjugates formed when formaldehyde reacted with GSH using liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS) coupled with an isotope dilution method. The results showed for the first time that (S)-1-(((R)-2-amino-3-(carboxymethylamino)-3-oxopropylthio)methyl)-5-oxopyrrolidine-2-carboxylic acid (PGF) and thioproline-glycine (SPro-Gly) are major metabolites in both nonenzymatic reactions and formaldehyde-exposed human cells. In particular, over 35% of the formaldehyde from external sources was found to convert to SPro-Gly in the exposed cells. Interestingly, data showed that these exposure-induced adducts exhibited good antioxidative properties, which can protect cells from hydrogen peroxide mediated oxidative insult. It is anticipated that the findings of this study could shed light on developing PGF and SPro-Gly as dietary supplements and on the development of noninvasive methods to assess health risks associated with formaldehyde exposure.

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“…1.1 to 2.2 µg based on the aerosol data and the average e-liquid consumption of 1.2 g per day (Landmesser et al 2019 ). Unfortunately, the labeled biomarkers of AA exposure, MTCA and MTCG, respectively, could not be determined due to insufficient long-term stability in urine of only 2 months (Landmesser et al 2020 ). Thus, MTCA and MTCG are not suited to assess AA exposure from smoking and vaping.…”

Section: Discussionmentioning

confidence: 99%

“…The specific biomarkers TCA and TCG for FA as well as MTCA and MTCG for AA were determined according to the fully validated method published by Landmesser et al ( 2020 ). Briefly, the biomarkers were cleaned up from major matrix components by solid-phase extraction followed by derivatization under alkaline conditions using propyl chloroformate.…”

Section: Methodsmentioning

confidence: 99%

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Assessment of the potential vaping-related exposure to carbonyls and epoxides using stable isotope-labeled precursors in the e-liquid

Landmesser

Scherer

et al. 2021

Arch Toxicol

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The formation of carbonyls and epoxides in e-cigarette (EC) aerosol is possible due to heating of the liquid constituents. However, high background levels of these compounds have inhibited a clear assessment of exposure during use of ECs. An EC containing an e-liquid replaced with 10% of 13C-labeled propylene glycol and glycerol was used in a controlled use clinical study with 20 EC users. In addition, five smokers smoked cigarettes spiked with the described e-liquid. Seven carbonyls (formaldehyde, acetaldehyde, acrolein, acetone, crotonaldehyde, methacrolein, propionaldehyde) were measured in the aerosol and the mainstream smoke. Corresponding biomarkers of exposure were determined in the user’s urine samples. 13C-labeled formaldehyde, acetaldehyde and acrolein were found in EC aerosol, while all seven labeled carbonyls were detected in smoke. The labeled biomarkers of exposure to formaldehyde (13C-thiazolidine carboxylic acid and 13C-N-(1,3-thiazolidine-4-carbonyl)glycine), acrolein (13C3-3-hydroxypropylmercapturic acid) and glycidol (13C3-dihydroxypropylmercapturic acid) were present in the urine of vapers indicating an EC use-specific exposure to these toxicants. However, other sources than vaping contribute to a much higher extent by several orders of magnitude to the overall exposure of these toxicants. Comparing data for the native (unlabeled) and the labeled (exposure-specific) biomarkers revealed vaping as a minor source of user’s exposure to these toxicants while other carbonyls and epoxides were not detectable in the EC aerosol.

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A novel quantification method for sulfur-containing biomarkers of formaldehyde and acetaldehyde exposure in human urine and plasma samples

Cited by 8 publications

References 46 publications

Electronic Cigarette Solvents, JUUL E-Liquids, and Biomarkers of Exposure: In Vivo Evidence for Acrolein and Glycidol in E-Cig-Derived Aerosols

Electronic Cigarette Solvents, JUUL E-Liquids, and Biomarkers of Exposure: In Vivo Evidence for Acrolein and Glycidol in E-Cig-Derived Aerosols

LC-MS/MS Quantitation of Formaldehyde–Glutathione Conjugates as Biomarkers of Formaldehyde Exposure and Exposure-Induced Antioxidants: A New Look on an Old Topic

Assessment of the potential vaping-related exposure to carbonyls and epoxides using stable isotope-labeled precursors in the e-liquid

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