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Article ; Online: Evaluation of wastewater-based epidemiology of COVID-19 approaches in Singapore's 'closed-system' scenario: A long-term country-wide assessment.

Marques Dos Santos, Mauricius / Caixia, Li / Snyder, Shane Allen

2023 Volume 244, Page(s) 120406

Abstract: With the COVID-19 pandemic the use of WBE to track diseases spread has rapidly evolved into a widely applied strategy worldwide. However, many of the current studies lack the necessary systematic approach and supporting quality of epidemiological data to ...

Abstract	With the COVID-19 pandemic the use of WBE to track diseases spread has rapidly evolved into a widely applied strategy worldwide. However, many of the current studies lack the necessary systematic approach and supporting quality of epidemiological data to fully evaluate the effectiveness and usefulness of such methods. Use of WBE in a very low disease prevalence setting and for long-term monitoring has yet to be validated and it is critical for its intended use as an early warning system. In this study we seek to evaluate the sensitivity of WBE approaches under low prevalence of disease and ability to provide early warning. Two monitoring scenarios were used: (i) city wide monitoring (population 5,700,000) and (ii) community/localized monitoring (population 24,000 to 240,000). Prediction of active cases by WBE using multiple linear regression shows that a multiplexed qPCR approach with three gene targets has a significant advantage over single-gene monitoring approaches, with R
MeSH term(s)	Humans ; Wastewater-Based Epidemiological Monitoring ; COVID-19/epidemiology ; Pandemics ; Singapore/epidemiology ; Linear Models ; RNA, Viral
Chemical Substances	RNA, Viral
Language	English
Publishing date	2023-07-25
Publishing country	England
Document type	Journal Article
ZDB-ID	202613-2
ISSN	1879-2448 ; 0043-1354
ISSN (online)	1879-2448
ISSN	0043-1354
DOI	10.1016/j.watres.2023.120406
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Article ; Online: Evaluation of wastewater-based epidemiology of COVID-19 approaches in Singapore's ‘closed-system’ scenario: A long-term country-wide assessment

Marques dos Santos, Mauricius / Caixia, Li / Snyder, Shane Allen

Water Research. 2023 Oct., v. 244 p.120406-

2023

Abstract	With the COVID-19 pandemic the use of WBE to track diseases spread has rapidly evolved into a widely applied strategy worldwide. However, many of the current studies lack the necessary systematic approach and supporting quality of epidemiological data to fully evaluate the effectiveness and usefulness of such methods. Use of WBE in a very low disease prevalence setting and for long-term monitoring has yet to be validated and it is critical for its intended use as an early warning system. In this study we seek to evaluate the sensitivity of WBE approaches under low prevalence of disease and ability to provide early warning. Two monitoring scenarios were used: (i) city wide monitoring (population 5,700,000) and (ii) community/localized monitoring (population 24,000 to 240,000). Prediction of active cases by WBE using multiple linear regression shows that a multiplexed qPCR approach with three gene targets has a significant advantage over single-gene monitoring approaches, with R² = 0.832 (RMSE 0.053) for an analysis using N, ORF1ab and S genes (R² = 0.677 to 0.793 for single gene strategies). A predicted disease prevalence of 0.001% (1 in 100,000) for a city-wide monitoring was estimated by the multiplexed RT-qPCR approach and was corroborated by epidemiological data evidence in three ‘waves’. Localized monitoring setting shows an estimated detectable disease prevalence of ∼0.002% (1 in 56,000) and is supported by the geospatial distribution of active cases and local population dynamics data. Data analysis also shows that this approach has a limitation in sensitivity, or hit rate, of 62.5 % and an associated high miss rate (false negative rate) of 37.5 % when compared to available epidemiological data. Nevertheless, our study shows that, with enough sampling resolution, WBE at a community level can achieve high precision and accuracies for case detection (96 % and 95 %, respectively) with low false omission rate (4.5 %) even at low disease prevalence levels.
Keywords	COVID-19 infection ; Singapore ; disease prevalence ; genes ; population dynamics ; prediction ; regression analysis ; research ; water ; Wastewater-based epidemiology (WBE) ; COVID-19 ; Multiplexed RT-qPCR ; SARS-CoV-2 ; Wastewater monitoring ; Pathogen detection
Language	English
Dates of publication	2023-10
Publishing place	Elsevier Ltd
Document type	Article ; Online
ZDB-ID	202613-2
ISSN	1879-2448 ; 0043-1354
ISSN (online)	1879-2448
ISSN	0043-1354
DOI	10.1016/j.watres.2023.120406
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Article ; Online: Analogy or fallacy, unsafe chemical alternatives: mechanistic insights into energy metabolism dysfunction induced by Bisphenol analogs in HepG2 cells

Jia, Shenglan / Marques Dos Santos, Mauricius / Li, Caixia / Fang, Mingliang / Mithusha, Sureshkumar / Snyder, Shane A.

Environment International. 2023 Apr. 20, p.107942-

2023 , Page(s) 107942–

Abstract: Bisphenol analogs (BPs) are widely used as industrial alternatives for Bisphenol A (BPA). Their toxicity assessment in humans has mainly focused on estrogenic activity, while other toxicity effects and mechanisms resulting from BPs exposure remain ... ...

Abstract	Bisphenol analogs (BPs) are widely used as industrial alternatives for Bisphenol A (BPA). Their toxicity assessment in humans has mainly focused on estrogenic activity, while other toxicity effects and mechanisms resulting from BPs exposure remain unclear. In this study, we investigated the effects of three BPs (Bisphenol AF (BPAF), Bisphenol G (BPG) and Bisphenol PH (BPPH)) on metabolic pathways of HepG2 cells. Results from comprehensive cellular bioenergetics analysis and nontarget metabolomics indicated that the most important process affected by BPs exposure was energy metabolism, as evidenced by reduced mitochondrial function and enhanced glycolysis. Compared to the control group, BPG and BPPH exhibited a consistent pattern of metabolic dysregulation, while BPAF differed from both, such as an increased ATP: ADP ratio (1.29-fold, p < 0.05) observed in BPAF and significantly decreased ATP: ADP ratio for BPG (0.28-fold, p < 0.001) and BPPH (0.45-fold, p < 0.001). Bioassay endpoint analysis revealed BPG/BPPH induced alterations in mitochondrial membrane potential and overproductions of reactive oxygen species. Taken together these data suggested that BPG/BPPH induced oxidative stress and mitochondrial damage in cells results in energy metabolism dysregulation. By contrast, BPAF had no effect on mitochondrial health, but induced a proliferation promoting effect on cells, which might contribute to the energy metabolism dysfunction. Interestingly, BPPH induced the greatest mitochondrial damage among the three BPs but did not exhibit Estrogen receptor alpha (ERα) activating effects. This study characterized the distinct metabolic mechanisms underlying energy metabolism dysregulation induced by different BPs in target human cells, providing new insight into the evaluation of the emerging BPA substitutes.
Keywords	bioassays ; bisphenol A ; bisphenol AF ; energy metabolism ; environment ; estrogen receptors ; estrogenic properties ; glycolysis ; humans ; membrane potential ; metabolomics ; mitochondria ; mitochondrial membrane ; oxidative stress ; reactive oxygen species ; toxicity ; bisphenol analogues ; global metabolomics ; cell proliferation
Language	English
Dates of publication	2023-0420
Publishing place	Elsevier Ltd
Document type	Article ; Online
Note	Pre-press version ; Use and reproduction
ZDB-ID	554791-x
ISSN	1873-6750 ; 0160-4120
ISSN (online)	1873-6750
ISSN	0160-4120
DOI	10.1016/j.envint.2023.107942
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Article: Recent advances in mass spectrometry analytical techniques for per- and polyfluoroalkyl substances (PFAS)

Jia, Shenglan / Marques Dos Santos, Mauricius / Li, Caixia / Snyder, Shane A.

Analytical and bioanalytical chemistry. 2022 Apr., v. 414, no. 9

2022

Abstract: The ubiquitous presence of per- and polyfluoroalkyl substances (PFAS) in various environments has led to increasing concern, and these chemicals have been confirmed as global contaminants. Following the chemical regulatory restrictions imposed, PFAS ... ...

Abstract	The ubiquitous presence of per- and polyfluoroalkyl substances (PFAS) in various environments has led to increasing concern, and these chemicals have been confirmed as global contaminants. Following the chemical regulatory restrictions imposed, PFAS alternatives that are presumed to be less toxic have been manufactured to replace the traditional ones in the market. However, owing to the original release and alternative usage, continuous accumulation of PFAS has been reported in environmental and human samples, with uncertain consequences for ecosystem and human health. It is crucial to promote and improve existing analytical techniques to facilitate the detection of trace amounts of PFAS in diverse environmental matrices. This review summarizes analytical methods that have been applied to and advanced for targeted detection and suspect screening of PFAS, which mainly include (i) sampling and sample preparation methods for various environment matrices and organisms, and quality assurance/quality control during the analysis process, and (ii) quantitative methods for targeted analysis and automated suspect screening strategies for non-targeted PFAS analysis, together with their applications, advantages, shortcomings, and need for new method development.
Keywords	analytical chemistry ; ecosystems ; human health ; humans ; markets ; mass spectrometry ; quality control ; toxicity
Language	English
Dates of publication	2022-04
Size	p. 2795-2807.
Publishing place	Springer Berlin Heidelberg
Document type	Article
Note	Review
ISSN	1618-2642
DOI	10.1007/s00216-022-03905-y
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Article: Non-targeted metabolomics revealing the effects of bisphenol analogues on human liver cancer cells

Jia, Shenglan / Li, Caixia / Fang, Mingliang / Marques Dos Santos, Mauricius / Snyder, Shane A.

Chemosphere. 2022 June, v. 297

2022

Abstract: Bisphenol analogues (BPs) are widely used in plastics, food packaging and other commercial products as non safer alternative of BPA. As emerging environmental contaminants, BPs have received considerable attention for their adverse effects on human ... ...

Abstract	Bisphenol analogues (BPs) are widely used in plastics, food packaging and other commercial products as non safer alternative of BPA. As emerging environmental contaminants, BPs have received considerable attention for their adverse effects on human health. However, their effects on liver metabolisms are only marginally understood. In this study, high-resolution mass spectrometry-based global metabolomics and extracellular flux (XF) analysis were applied to characterize the cellular metabolome alterations and reveal the possible mechanisms of the metabolic disorders associated with BPs-induced toxicity in HepG2 cells. BPE, BPB and BPAP with similar chemical structures were selected to compare their interference with different metabolic pathways. A total of 61 key metabolite profiles were significantly altered after exposure to the three BPs. Overall, BPs altered metabolites which are associated with energy metabolism, oxidative stress, cell proliferation and nucleotides synthesis. The primary dysregulated pathways included energy and nucleotides synthesis related Purine and Glycolysis/Gluconeogenesis metabolism. In addition, attenuated mitochondrial function and enhanced glycolysis were found under BPB and BPAP treatment. While attenuated glycolysis was observed under BPE treatment. These findings may provide potential biomarkers indicating the cytotoxicity of BPs and prompt a deeper understanding of the intramolecular metabolic processes induced by BPs exposure.
Keywords	biomarkers ; cell proliferation ; cytotoxicity ; energy ; energy metabolism ; gluconeogenesis ; glycolysis ; human health ; humans ; liver ; liver neoplasms ; mass spectrometry ; metabolites ; metabolome ; metabolomics ; mitochondria ; nucleotides ; oxidative stress ; pollution
Language	English
Dates of publication	2022-06
Publishing place	Elsevier Ltd
Document type	Article
ZDB-ID	120089-6
ISSN	1879-1298 ; 0045-6535 ; 0366-7111
ISSN (online)	1879-1298
ISSN	0045-6535 ; 0366-7111
DOI	10.1016/j.chemosphere.2022.134088
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Article ; Online: Recent advances in mass spectrometry analytical techniques for per- and polyfluoroalkyl substances (PFAS).

Jia, Shenglan / Marques Dos Santos, Mauricius / Li, Caixia / Snyder, Shane A

Analytical and bioanalytical chemistry

2022 Volume 414, Issue 9, Page(s) 2795–2807

Abstract	The ubiquitous presence of per- and polyfluoroalkyl substances (PFAS) in various environments has led to increasing concern, and these chemicals have been confirmed as global contaminants. Following the chemical regulatory restrictions imposed, PFAS alternatives that are presumed to be less toxic have been manufactured to replace the traditional ones in the market. However, owing to the original release and alternative usage, continuous accumulation of PFAS has been reported in environmental and human samples, with uncertain consequences for ecosystem and human health. It is crucial to promote and improve existing analytical techniques to facilitate the detection of trace amounts of PFAS in diverse environmental matrices. This review summarizes analytical methods that have been applied to and advanced for targeted detection and suspect screening of PFAS, which mainly include (i) sampling and sample preparation methods for various environment matrices and organisms, and quality assurance/quality control during the analysis process, and (ii) quantitative methods for targeted analysis and automated suspect screening strategies for non-targeted PFAS analysis, together with their applications, advantages, shortcomings, and need for new method development.
MeSH term(s)	Ecosystem ; Fluorocarbons/analysis ; Humans ; Mass Spectrometry ; Specimen Handling
Chemical Substances	Fluorocarbons
Language	English
Publishing date	2022-02-07
Publishing country	Germany
Document type	Journal Article ; Review
ZDB-ID	201093-8
ISSN	1618-2650 ; 0016-1152 ; 0372-7920
ISSN (online)	1618-2650
ISSN	0016-1152 ; 0372-7920
DOI	10.1007/s00216-022-03905-y
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Article ; Online: Non-targeted metabolomics revealing the effects of bisphenol analogues on human liver cancer cells.

Jia, Shenglan / Li, Caixia / Fang, Mingliang / Marques Dos Santos, Mauricius / Snyder, Shane A

Chemosphere

2022 Volume 297, Page(s) 134088

Abstract	Bisphenol analogues (BPs) are widely used in plastics, food packaging and other commercial products as non safer alternative of BPA. As emerging environmental contaminants, BPs have received considerable attention for their adverse effects on human health. However, their effects on liver metabolisms are only marginally understood. In this study, high-resolution mass spectrometry-based global metabolomics and extracellular flux (XF) analysis were applied to characterize the cellular metabolome alterations and reveal the possible mechanisms of the metabolic disorders associated with BPs-induced toxicity in HepG2 cells. BPE, BPB and BPAP with similar chemical structures were selected to compare their interference with different metabolic pathways. A total of 61 key metabolite profiles were significantly altered after exposure to the three BPs. Overall, BPs altered metabolites which are associated with energy metabolism, oxidative stress, cell proliferation and nucleotides synthesis. The primary dysregulated pathways included energy and nucleotides synthesis related Purine and Glycolysis/Gluconeogenesis metabolism. In addition, attenuated mitochondrial function and enhanced glycolysis were found under BPB and BPAP treatment. While attenuated glycolysis was observed under BPE treatment. These findings may provide potential biomarkers indicating the cytotoxicity of BPs and prompt a deeper understanding of the intramolecular metabolic processes induced by BPs exposure.
MeSH term(s)	Benzhydryl Compounds/analysis ; Benzhydryl Compounds/toxicity ; Hep G2 Cells ; Humans ; Liver Neoplasms ; Metabolome ; Metabolomics ; Nucleotides
Chemical Substances	Benzhydryl Compounds ; Nucleotides
Language	English
Publishing date	2022-02-22
Publishing country	England
Document type	Journal Article
ZDB-ID	120089-6
ISSN	1879-1298 ; 0045-6535 ; 0366-7111
ISSN (online)	1879-1298
ISSN	0045-6535 ; 0366-7111
DOI	10.1016/j.chemosphere.2022.134088
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Article ; Online: Comparison of monochloramination and chlorination of 1,3-diphenylguandine (DPG): Kinetics, transformation products, and cell-based in-vitro testing.

Ying, Lebing / Marques Dos Santos, Mauricius / Jia, Shenglan / Li, Caixia / Lee, Theodora H Y / Mensah, Anette Tele / Snyder, Shane Allen

The Science of the total environment

2023 Volume 906, Page(s) 167743

Abstract: As a widely used secondary vulcanization accelerator in the rubber industry, 1,3-diphenylguanidine (DPG) poses risks to human health and the environment. To compare and comprehend the disinfection process of DPG, this work investigates the reaction ... ...

Abstract	As a widely used secondary vulcanization accelerator in the rubber industry, 1,3-diphenylguanidine (DPG) poses risks to human health and the environment. To compare and comprehend the disinfection process of DPG, this work investigates the reaction kinetics, toxicity, and transformation products (TPs) of DPG during chlorination and monochloramination. It has been revealed that the reactivity of monochloramine is significantly slower compared to chlorination of DPG, with the maximum efficiency observed at pH 7 to pH 8. Cytotoxicity assessment using HepG2 and THP-1 cells reveals that cytotoxicity hierarchy is as follows: chlorine TPs > monochloramine TPs > DPG. Moreover, oxidant-to-DPG molar ratios 10 and 20 lead to higher cytotoxicity in both chlorination and monochloramination compared to ratio 5 and 100. Additionally, cell bioenergetics experiments demonstrate that chlorine and monochloramine TPs induce mitochondrial dysfunction and enhance glycolytic function in HepG2 cells. The genotoxic response from p53 signaling further suggested genotoxic effects of certain TPs. Furthermore, analysis of TPs using high-resolution mass spectrometry (HRMS) identifies ten TPs, with chlorination yielding more TPs than monochloramination. Generally, a chlorine or monochloramine molar ratio to DPG of 10-20 results in an increased formation of TPs and heightened cytotoxicity. Notably, higher oxidant molar ratios increased the formation of monoguanidine TPs and DPG hydroxylation during chlorination, whereas monochloramination lead to DPG substitution predominantly generating chlorinated DPG due to weaker oxidation effects. These findings provide valuable information for the appropriate treatment of DPG and disinfection processes in water facilities to mitigate potential risks to human health and the ecosystem.
MeSH term(s)	Humans ; Halogenation ; Chlorine/chemistry ; Ecosystem ; Water Purification/methods ; Disinfection/methods ; Oxidants ; Water Pollutants, Chemical/analysis ; Kinetics
Chemical Substances	chloramine (KW8K411A1P) ; Chlorine (4R7X1O2820) ; Oxidants ; Water Pollutants, Chemical
Language	English
Publishing date	2023-10-12
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2023.167743
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Article ; Online: Formation of halogenated forms of bisphenol A (BPA) in water: Resolving isomers with ion mobility - mass spectrometry and the role of halogenation position in cellular toxicity.

Marques Dos Santos, Mauricius / Li, Caixia / Jia, Shenglan / Thomas, Mikael / Gallard, Hervé / Croué, Jean-Philippe / Carato, Pascal / Snyder, Shane Allen

Journal of hazardous materials

2023 Volume 465, Page(s) 133229

Abstract: Halogenated BPA (XBPA) forms resulting from water chlorination can lead to increased toxicity and different biological effects. While previous studies have reported the occurrence of different XBPAs, analytical limitation have hindered the analysis and ... ...

Abstract	Halogenated BPA (XBPA) forms resulting from water chlorination can lead to increased toxicity and different biological effects. While previous studies have reported the occurrence of different XBPAs, analytical limitation have hindered the analysis and differentiation of the many potential isomeric forms. Using online solid-phase extraction - liquid chromatography - ion-mobility - high-resolution mass spectrometry (OSPE-LC-IM-HRMS), we demonstrated a rapid analysis method for the analysis of XBPA forms after water chlorination, with a total analysis time of less than 10 min including extraction and concentration and low detection limits (∼5-80 ng/L range). A multi in-vitro bioassay testing approach for the identified products revealed that cytotoxicity and bioenergetics impacts were largely associated with the presence of halogen atoms at positions 2 or 2' and the overall number of halogens incorporated into the BPA molecule. Different XBPA also showed distinct impacts on oxidative stress, peroxisome proliferator-activated receptor gamma - PPARγ, and inflammatory response. While increased DNA damage was observed for chlorinated water samples (4.14 ± 1.21-fold change), the additive effect of the selected 20 XBPA studied could not explain the increased DNA damage observed, indicating that additional species or synergistic effects might be at play.
MeSH term(s)	Halogenation ; Disinfection/methods ; Drinking Water/analysis ; Halogens ; Water Purification/methods ; Mass Spectrometry ; Water Pollutants, Chemical/analysis ; Disinfectants/analysis ; Benzhydryl Compounds ; Phenols
Chemical Substances	bisphenol A (MLT3645I99) ; Drinking Water ; Halogens ; Water Pollutants, Chemical ; Disinfectants ; Benzhydryl Compounds ; Phenols
Language	English
Publishing date	2023-12-13
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	1491302-1
ISSN	1873-3336 ; 0304-3894
ISSN (online)	1873-3336
ISSN	0304-3894
DOI	10.1016/j.jhazmat.2023.133229
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Article ; Online: Analogy or fallacy, unsafe chemical alternatives: Mechanistic insights into energy metabolism dysfunction induced by Bisphenol analogs in HepG2 cells.

Jia, Shenglan / Marques Dos Santos, Mauricius / Li, Caixia / Fang, Mingliang / Sureshkumar, Mithusha / Snyder, Shane A

Environment international

2023 Volume 175, Page(s) 107942

Abstract	Bisphenol analogs (BPs) are widely used as industrial alternatives for Bisphenol A (BPA). Their toxicity assessment in humans has mainly focused on estrogenic activity, while other toxicity effects and mechanisms resulting from BPs exposure remain unclear. In this study, we investigated the effects of three BPs (Bisphenol AF (BPAF), Bisphenol G (BPG) and Bisphenol PH (BPPH)) on metabolic pathways of HepG2 cells. Results from comprehensive cellular bioenergetics analysis and nontarget metabolomics indicated that the most important process affected by BPs exposure was energy metabolism, as evidenced by reduced mitochondrial function and enhanced glycolysis. Compared to the control group, BPG and BPPH exhibited a consistent pattern of metabolic dysregulation, while BPAF differed from both, such as an increased ATP: ADP ratio (1.29-fold, p < 0.05) observed in BPAF and significantly decreased ATP: ADP ratio for BPG (0.28-fold, p < 0.001) and BPPH (0.45-fold, p < 0.001). Bioassay endpoint analysis revealed BPG/BPPH induced alterations in mitochondrial membrane potential and overproductions of reactive oxygen species. Taken together these data suggested that BPG/BPPH induced oxidative stress and mitochondrial damage in cells results in energy metabolism dysregulation. By contrast, BPAF had no effect on mitochondrial health, but induced a proliferation promoting effect on cells, which might contribute to the energy metabolism dysfunction. Interestingly, BPPH induced the greatest mitochondrial damage among the three BPs but did not exhibit Estrogen receptor alpha (ERα) activating effects. This study characterized the distinct metabolic mechanisms underlying energy metabolism dysregulation induced by different BPs in target human cells, providing new insight into the evaluation of the emerging BPA substitutes.
MeSH term(s)	Humans ; Adenosine Triphosphate ; Benzhydryl Compounds/toxicity ; Energy Metabolism/drug effects ; Hep G2 Cells
Chemical Substances	4,4'-hexafluorisopropylidene diphenol (OH7IX8A37J) ; Adenosine Triphosphate (8L70Q75FXE) ; Benzhydryl Compounds ; bisphenol A (MLT3645I99)
Language	English
Publishing date	2023-04-20
Publishing country	Netherlands
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	554791-x
ISSN	1873-6750 ; 0160-4120
ISSN (online)	1873-6750
ISSN	0160-4120
DOI	10.1016/j.envint.2023.107942
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