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Article: Mass spectrometric determination of N7-HPTE-dG and N7-HPTE-Gua in mammalian cells and mice exposed to methoxychlor, an emergent persistent organic pollutant

Wu, Jiabin / Wang, Fuyue / Xie, Guangshan / Cai, Zongwei

Journal of hazardous materials. 2022 June 15, v. 432

2022

Abstract: Methoxychlor (MXC) is an organopesticide classified as a “Proposed Persistent Organic Pollutant” in the Stockholm Convention, and recent studies revealed that MXC could induce DNA strand breaks, whereas its underlying mechanisms were underinvestigated. ... ...

Abstract	Methoxychlor (MXC) is an organopesticide classified as a “Proposed Persistent Organic Pollutant” in the Stockholm Convention, and recent studies revealed that MXC could induce DNA strand breaks, whereas its underlying mechanisms were underinvestigated. Here, we first reported that hydroxymethoxychlor (HPTE), one of MXC’s active metabolites, could be oxidized in vivo to form quinone intermediate, which attacked N7 position of 2′-deoxyguanosine to form N7-HPTE-deoxyguanosine (N7-HPTE-dG), followed by depurination to produce N7-HPTE-guanine (N7-HPTE-Gua) in MXC-treated mammalian cells and tissues from mice fed with MXC, employing an ultra-performance liquid chromatography-electrospray ionization-tandem mass spectrometry (UPLC-ESI-MS/MS) method. We observed a positive correlation between the doses of MXC exposure and the levels of N7-HPTE-Gua and N7-HPTE-dG in cytoplasm and genomic DNA, respectively. Furthermore, after removal of exogenous MXC, the amount of genomic N7-HPTE-dG was significantly decreased during 24 h, while the level of cytoplasmic N7-HPTE-Gua was elevated during first 12 h, indicating the accumulation of the N7-HPTE-Gua in cells. Additionally, for animal experiment, genomic N7-HPTE-dG was observed in livers and cortexes from female C57BL/6 mice fed with MXC, suggesting a potential mechanism of its hepatoxicity and neurotoxicity. Overall, our study provides new understanding about the formation of MXC-induced DNA adducts in mammalian cells and animal models.
Keywords	DNA adducts ; animal experimentation ; cytoplasm ; females ; genomics ; metabolites ; methoxychlor ; neurotoxicity ; persistent organic pollutants ; quinones
Language	English
Dates of publication	2022-0615
Publishing place	Elsevier B.V.
Document type	Article
ZDB-ID	1491302-1
ISSN	1873-3336 ; 0304-3894
ISSN (online)	1873-3336
ISSN	0304-3894
DOI	10.1016/j.jhazmat.2022.128741
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Mass spectrometric determination of N7-HPTE-dG and N7-HPTE-Gua in mammalian cells and mice exposed to methoxychlor, an emergent persistent organic pollutant.

Wu, Jiabin / Wang, Fuyue / Xie, Guangshan / Cai, Zongwei

Journal of hazardous materials

2022 Volume 432, Page(s) 128741

Abstract: Methoxychlor (MXC) is an organopesticide classified as a "Proposed Persistent Organic Pollutant" in the Stockholm Convention, and recent studies revealed that MXC could induce DNA strand breaks, whereas its underlying mechanisms were underinvestigated. ... ...

Abstract	Methoxychlor (MXC) is an organopesticide classified as a "Proposed Persistent Organic Pollutant" in the Stockholm Convention, and recent studies revealed that MXC could induce DNA strand breaks, whereas its underlying mechanisms were underinvestigated. Here, we first reported that hydroxymethoxychlor (HPTE), one of MXC's active metabolites, could be oxidized in vivo to form quinone intermediate, which attacked N7 position of 2'-deoxyguanosine to form N7-HPTE-deoxyguanosine (N7-HPTE-dG), followed by depurination to produce N7-HPTE-guanine (N7-HPTE-Gua) in MXC-treated mammalian cells and tissues from mice fed with MXC, employing an ultra-performance liquid chromatography-electrospray ionization-tandem mass spectrometry (UPLC-ESI-MS/MS) method. We observed a positive correlation between the doses of MXC exposure and the levels of N7-HPTE-Gua and N7-HPTE-dG in cytoplasm and genomic DNA, respectively. Furthermore, after removal of exogenous MXC, the amount of genomic N7-HPTE-dG was significantly decreased during 24 h, while the level of cytoplasmic N7-HPTE-Gua was elevated during first 12 h, indicating the accumulation of the N7-HPTE-Gua in cells. Additionally, for animal experiment, genomic N7-HPTE-dG was observed in livers and cortexes from female C57BL/6 mice fed with MXC, suggesting a potential mechanism of its hepatoxicity and neurotoxicity. Overall, our study provides new understanding about the formation of MXC-induced DNA adducts in mammalian cells and animal models.
MeSH term(s)	Animals ; DNA Adducts ; Deoxyguanosine ; Female ; Mammals/metabolism ; Methoxychlor/toxicity ; Mice ; Mice, Inbred C57BL ; Persistent Organic Pollutants ; Phenols/toxicity ; Tandem Mass Spectrometry
Chemical Substances	DNA Adducts ; Phenols ; Deoxyguanosine (G9481N71RO) ; Methoxychlor (RIA79UD69L)
Language	English
Publishing date	2022-03-22
Publishing country	Netherlands
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1491302-1
ISSN	1873-3336 ; 0304-3894
ISSN (online)	1873-3336
ISSN	0304-3894
DOI	10.1016/j.jhazmat.2022.128741
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Article: Metabolomics and proteomics study reveals the effects of benzo[a]pyrene on the viability and migration of KYSE-150 esophageal cells

Shen, Yuting / Xie, Guangshan / Lin, Siyi / Zhu, Lin / Zhang, Hongna / Yang, Zhu / Cai, Zongwei

Science of the total environment. 2022 June 10, v. 824

2022

Abstract: A representative polycyclic aromatic hydrocarbon, benzo[a]pyrene (B[a]P), has been widely detected in environmental compartments and is highly carcinogenic to humans. Oral ingestion of B[a]P is the dominant exposure pathway. The esophagus acts as the ... ...

Abstract	A representative polycyclic aromatic hydrocarbon, benzo[a]pyrene (B[a]P), has been widely detected in environmental compartments and is highly carcinogenic to humans. Oral ingestion of B[a]P is the dominant exposure pathway. The esophagus acts as the first contact point when B[a]P enters the human body. However, its role in the development of human esophageal cancer is rarely discussed. Herein, we employed untargeted metabolomics in combination with proteomics to explore B[a]P-related intracellular responses in human esophageal cell lines. Our results demonstrated that B[a]P exposure induced significant metabolic disorders, further leading to overproduction of reactive oxygen species (ROS) and disturbance of the cellular viability process and migration ability of esophageal cells. In response, glutathione (GSH) was consumed to meet the demand for cellular detoxification, and thioredoxin (TXN) was upregulated to balance the cellular redox. These alterations caused the reregulation of some specific protein families, including S100A proteins, ribosomal proteins, and histone H1 proteins. Such changes impeded the viability and migration of esophageal cells, which could adversely affect wound healing of the epithelium. These cellular responses indicate that B[a]P will cause serious cellular damage to esophageal cells and increase the carcinogenic risk even as a result of short-term exposure. Our omics study demonstrated how benzo[a]pyrene hampered the migration of esophageal cells and proposed a plausible mechanism underlying its carcinogenicity, which may contribute to our understanding of environmental pollutants.
Keywords	acute exposure ; carcinogenicity ; cell viability ; environment ; epithelium ; esophageal neoplasms ; esophagus ; glutathione ; histones ; humans ; metabolomics ; polycyclic aromatic hydrocarbons ; proteomics ; reactive oxygen species ; risk ; thioredoxins
Language	English
Dates of publication	2022-0610
Publishing place	Elsevier B.V.
Document type	Article
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2022.153761
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Article: [Synthesis of zwitterionic dual-functional metal-organic framework nanocomposite with ultra-hydrophilicity for selective enrichment of glycopeptides].

Li, Dapeng / Xie, Guangshan / Xie, Peisi / Zhu, Lin / Cai, Zongwei

Se pu = Chinese journal of chromatography

2021 Volume 39, Issue 3, Page(s) 205–210

Abstract: Protein glycosylation is a ubiquitous and important biological process involved in various molecular functions and biological pathways. It also yields important biomarkers for clinical diagnoses. However, glycopeptide analysis is challenging due to low ... ...

Abstract	Protein glycosylation is a ubiquitous and important biological process involved in various molecular functions and biological pathways. It also yields important biomarkers for clinical diagnoses. However, glycopeptide analysis is challenging due to low abundance, low ionization efficiency, and glycan heterogeneity. In the present study, a method based on hydrophilic interaction liquid chromatography (HILIC) was developed for the selective enrichment of glycopeptides using a novel metal-organic framework (MOF) nanocomposite (AuGC/ZIF-8). Dual functionalization with glutathione and cysteine has resulted in an ultra-hydrophilic MOF, with synergistic effects and lower steric hindrance, providing more affinity sites for the glycopeptide enrichment. Horseradish peroxidase (HRP) was used as a model glycoprotein, and AuGC/ZIF-8 was used to enrich glycopeptides prior to analysis by matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF MS). AuGC/ZIF-8 displayed outstanding performance at enriching HRP glycopeptides, with high enrichment capacity (250 μg/mg), high selectivity in mixtures containing bovine serum albumin (BSA) (HRP-BSA (1∶200, mass ratio)), and high sensitivity at very low content (0.3 ng/μL). Thus this MOF holds promise for in-depth, comprehensive glycoproteomic and related analysis.
MeSH term(s)	Chromatography, Liquid ; Glycopeptides/chemistry ; Horseradish Peroxidase ; Hydrophobic and Hydrophilic Interactions ; Metal-Organic Frameworks/chemistry ; Nanocomposites ; Serum Albumin, Bovine ; Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization
Chemical Substances	Glycopeptides ; Metal-Organic Frameworks ; Serum Albumin, Bovine (27432CM55Q) ; Horseradish Peroxidase (EC 1.11.1.-)
Language	Chinese
Publishing date	2021-07-05
Publishing country	China
Document type	Journal Article
ISSN	1000-8713
ISSN	1000-8713
DOI	10.3724/SP.J.1123.2020.11006
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Article ; Online: Metabolomics and proteomics study reveals the effects of benzo[a]pyrene on the viability and migration of KYSE-150 esophageal cells.

Shen, Yuting / Xie, Guangshan / Lin, Siyi / Zhu, Lin / Zhang, Hongna / Yang, Zhu / Cai, Zongwei

The Science of the total environment

2022 Volume 824, Page(s) 153761

Abstract	A representative polycyclic aromatic hydrocarbon, benzo[a]pyrene (B[a]P), has been widely detected in environmental compartments and is highly carcinogenic to humans. Oral ingestion of B[a]P is the dominant exposure pathway. The esophagus acts as the first contact point when B[a]P enters the human body. However, its role in the development of human esophageal cancer is rarely discussed. Herein, we employed untargeted metabolomics in combination with proteomics to explore B[a]P-related intracellular responses in human esophageal cell lines. Our results demonstrated that B[a]P exposure induced significant metabolic disorders, further leading to overproduction of reactive oxygen species (ROS) and disturbance of the cellular viability process and migration ability of esophageal cells. In response, glutathione (GSH) was consumed to meet the demand for cellular detoxification, and thioredoxin (TXN) was upregulated to balance the cellular redox. These alterations caused the reregulation of some specific protein families, including S100A proteins, ribosomal proteins, and histone H1 proteins. Such changes impeded the viability and migration of esophageal cells, which could adversely affect wound healing of the epithelium. These cellular responses indicate that B[a]P will cause serious cellular damage to esophageal cells and increase the carcinogenic risk even as a result of short-term exposure. SYNOPSIS: Our omics study demonstrated how benzo[a]pyrene hampered the migration of esophageal cells and proposed a plausible mechanism underlying its carcinogenicity, which may contribute to our understanding of environmental pollutants.
MeSH term(s)	Benzo(a)pyrene/metabolism ; Benzo(a)pyrene/toxicity ; Carcinogens ; Esophagus/metabolism ; Glutathione ; Humans ; Metabolomics ; Polycyclic Aromatic Hydrocarbons ; Proteomics
Chemical Substances	Carcinogens ; Polycyclic Aromatic Hydrocarbons ; Benzo(a)pyrene (3417WMA06D) ; Glutathione (GAN16C9B8O)
Language	English
Publishing date	2022-02-11
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.2022.153761
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Article ; Online: Long-term percutaneous triclosan exposure induces thyroid damage in mice: Interpretation of toxicity mechanism from metabolic and proteomic perspectives.

Liang, Yanshan / Li, Leiguang / Zhang, Hongna / Dai, Qingyuan / Xie, Guangshan / Lei, Bo / Yang, Zhu / Cai, Zongwei

Journal of hazardous materials

2023 Volume 454, Page(s) 131532

Abstract: Triclosan (TCS) is an antiseptic incorporated in consumer goods and personal care products that can be absorbed via the skin, raising public health concerns for its continuous detection in human biofluids and tissues. Epidemiology has associated TCS ... ...

Abstract	Triclosan (TCS) is an antiseptic incorporated in consumer goods and personal care products that can be absorbed via the skin, raising public health concerns for its continuous detection in human biofluids and tissues. Epidemiology has associated TCS exposure with thyroid function disturbances and decreasing serum thyroid hormone (TH) levels, but the underlying mechanism remains unclear. In this study, we revealed hypothyroidism and histological alternation in the thyroid of mice with chronic percutaneous exposure to TCS, indicating a TCS-caused thyroid impairment. Subsequently, multi-omics approaches were performed to investigate the molecular mechanism of the thyroid in response to long-term dermal TCS exposure. We discovered that TCS interfered with the TH synthesis as indicated by the changes in the levels of the synthetic materials for TH (iodide, Tg, and H
MeSH term(s)	Animals ; Humans ; Mice ; Anti-Infective Agents, Local/toxicity ; Hydrogen Peroxide ; Proteomics ; Thyroid Gland ; Thyroid Hormones ; Triclosan/toxicity
Chemical Substances	Anti-Infective Agents, Local ; Hydrogen Peroxide (BBX060AN9V) ; Thyroid Hormones ; Triclosan (4NM5039Y5X)
Language	English
Publishing date	2023-04-28
Publishing country	Netherlands
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1491302-1
ISSN	1873-3336 ; 0304-3894
ISSN (online)	1873-3336
ISSN	0304-3894
DOI	10.1016/j.jhazmat.2023.131532
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Article: Comprehensive multi-omics approaches reveal the hepatotoxic mechanism of perfluorohexanoic acid (PFHxA) in mice

Jiang, Lilong / Hong, Yanjun / Xie, Guangshan / Zhang, Jinghui / Zhang, Hongna / Cai, Zongwei

Science of the total environment. 2021 Oct. 10, v. 790

2021

Abstract: Perfluorohexanoic acid (PFHxA), one of the short-chain perfluoroalkyl acids (PFAAs), is considered as a substitute of perfluorooctane sulfonate (PFOS). This emerging organic pollutant is persistent and highly bioavailable to humans, raising concerns ... ...

Abstract	Perfluorohexanoic acid (PFHxA), one of the short-chain perfluoroalkyl acids (PFAAs), is considered as a substitute of perfluorooctane sulfonate (PFOS). This emerging organic pollutant is persistent and highly bioavailable to humans, raising concerns about its potential health risks. There are currently few researches on the toxicity of PFHxA. Liver has been suggested to be the main target of PFHxA toxicity, and the mechanism remains unclear. Herein, we investigated the transcriptomic, proteomic, and metabolomic landscape in PFHxA-exposed mice. Using these approaches, we identified several valuable biological processes involved in the process of liver injury, comprising fatty acid biosynthesis and degradation pathways, which might be induced by peroxisome proliferator-activated receptor (PPAR) signaling pathway. These processes further promoted oxidative stress and induced liver injury. Meanwhile, abnormalities in purine metabolism and glutathione metabolism were observed during the liver injury induced by PFHxA, indicating the production of oxidative stress. Finally, our present multi-omics studies provided new insights into the mechanisms involved in PFHxA-induced liver injury.
Keywords	bioavailability ; biosynthesis ; environment ; glutathione ; hepatotoxicity ; landscapes ; liver ; metabolomics ; multiomics ; oxidative stress ; perfluorohexanoic acid ; perfluorooctane sulfonic acid ; peroxisome proliferator-activated receptors ; pollutants ; proteomics ; transcriptomics
Language	English
Dates of publication	2021-1010
Publishing place	Elsevier B.V.
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2021.148160
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Article ; Online: Comprehensive multi-omics approaches reveal the hepatotoxic mechanism of perfluorohexanoic acid (PFHxA) in mice.

Jiang, Lilong / Hong, Yanjun / Xie, Guangshan / Zhang, Jinghui / Zhang, Hongna / Cai, Zongwei

The Science of the total environment

2021 Volume 790, Page(s) 148160

Abstract	Perfluorohexanoic acid (PFHxA), one of the short-chain perfluoroalkyl acids (PFAAs), is considered as a substitute of perfluorooctane sulfonate (PFOS). This emerging organic pollutant is persistent and highly bioavailable to humans, raising concerns about its potential health risks. There are currently few researches on the toxicity of PFHxA. Liver has been suggested to be the main target of PFHxA toxicity, and the mechanism remains unclear. Herein, we investigated the transcriptomic, proteomic, and metabolomic landscape in PFHxA-exposed mice. Using these approaches, we identified several valuable biological processes involved in the process of liver injury, comprising fatty acid biosynthesis and degradation pathways, which might be induced by peroxisome proliferator-activated receptor (PPAR) signaling pathway. These processes further promoted oxidative stress and induced liver injury. Meanwhile, abnormalities in purine metabolism and glutathione metabolism were observed during the liver injury induced by PFHxA, indicating the production of oxidative stress. Finally, our present multi-omics studies provided new insights into the mechanisms involved in PFHxA-induced liver injury.
MeSH term(s)	Alkanesulfonic Acids ; Animals ; Caproates/toxicity ; Environmental Pollutants/toxicity ; Fluorocarbons/analysis ; Fluorocarbons/toxicity ; Mice ; Proteomics
Chemical Substances	Alkanesulfonic Acids ; Caproates ; Environmental Pollutants ; Fluorocarbons ; perfluorohexanoic acid (ZP34Q2220R)
Language	English
Publishing date	2021-05-31
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.2021.148160
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Article ; Online: Evaluation of nanoplastics toxicity in the soil nematode Caenorhabditis elegans by iTRAQ-based quantitative proteomics.

Huang, Gefei / Ma, Yiming / Xie, Dongying / Zhao, Cunmin / Zhu, Lin / Xie, Guangshan / Wu, Pengfei / Wang, Wei / Zhao, Zhongying / Cai, Zongwei

The Science of the total environment

2022 , Page(s) 160646

Abstract: Plastic pollution is recognized as a major threat to ecosystems in the 21st century. Large plastic objects undergo biotic and abiotic degradation to generate micro- and nano-sized plastic pieces. Despite tremendous efforts to evaluate the adverse effects ...

Abstract	Plastic pollution is recognized as a major threat to ecosystems in the 21st century. Large plastic objects undergo biotic and abiotic degradation to generate micro- and nano-sized plastic pieces. Despite tremendous efforts to evaluate the adverse effects of microplastics, a comprehensive understanding of the toxicity of nanoplastics remains elusive, especially at the protein level. To this end, we used isobaric-tag-for-relative-and-absolute-quantitation-based quantitative proteomics to investigate the proteome dynamics of the soil nematode Caenorhabditis elegans in response to exposure to 100 nm polystyrene nanoplastics (PS-NPs). After 48 h of exposure to 0.1, 1, or 10 mg/L PS-NPs, 136 out of 1684 proteins were differentially expressed and 108 of these proteins were upregulated. These proteins were related to ribosome biogenesis, translation, proteolysis, kinases, protein processing in the endoplasmic reticulum, and energy metabolism. Remarkably, changes in proteome dynamics in response to exposure to PS-NPs were consistent with the phenotypic defects of C. elegans. Collectively, our findings demonstrate that disruption of proteome homeostasis is a biological consequence of PS-NPs accumulation in C. elegans, which provides insights into the molecular mechanisms underlying the toxicology of nanoplastics.
Language	English
Publishing date	2022-12-06
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.2022.160646
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Article ; Online: Identification of Lysine Acetylation Sites on MERS-CoV Replicase pp1ab.

Zhu, Lin / Fung, Sin-Yee / Xie, Guangshan / Wong, Lok-Yin Roy / Jin, Dong-Yan / Cai, Zongwei

Molecular & cellular proteomics : MCP

2020 Volume 19, Issue 8, Page(s) 1303–1309

Abstract: MERS is a life-threatening disease and MERS-CoV has the potential to cause the next pandemic. Protein acetylation is known to play a crucial role in host response to viral infection. Acetylation of viral proteins encoded by other RNA viruses have been ... ...

Abstract	MERS is a life-threatening disease and MERS-CoV has the potential to cause the next pandemic. Protein acetylation is known to play a crucial role in host response to viral infection. Acetylation of viral proteins encoded by other RNA viruses have been reported to affect viral replication. It is therefore of interest to see whether MERS-CoV proteins are also acetylated. Viral proteins obtained from infected cells were trypsin-digested into peptides. Acetylated peptides were enriched by immunoprecipitation and subject to nano-LC-Orbitrap analysis. Bioinformatic analysis was performed to assess the conservation level of identified acetylation sites and to predict the upstream regulatory factors. A total of 12 acetylation sites were identified from 7 peptides, which all belong to the replicase polyprotein pp1ab. All identified acetylation sites were found to be highly conserved across MERS-CoV sequences in NCBI database. Upstream factors, including deacetylases of the SIRT1 and HDAC families as well as acetyltransferases of the TIP60 family, were predicted to be responsible for regulating the acetylation events identified. Western blotting confirms that acetylation events indeed occur on pp1ab protein by expressing NSP4 in HEK293 cells. Acetylation events on MERS-CoV viral protein pp1ab were identified for the first time, which indicate that MERS-CoV might use the host acetylation machinery to regulate its enzyme activity and to achieve optimal replication. Upstream factors were predicted, which might facilitate further analysis of the regulatory mechanism of MERS-CoV replication.
MeSH term(s)	Acetylation ; HEK293 Cells ; Humans ; Lysine/metabolism ; Middle East Respiratory Syndrome Coronavirus/metabolism ; Viral Proteins/metabolism
Chemical Substances	Viral Proteins ; Lysine (K3Z4F929H6)
Keywords	covid19
Language	English
Publishing date	2020-05-18
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	2075924-1
ISSN	1535-9484 ; 1535-9476
ISSN (online)	1535-9484
ISSN	1535-9476
DOI	10.1074/mcp.RA119.001897
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