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1.
Nature ; 612(7939): 246-251, 2022 12.
Artículo en Inglés | MEDLINE | ID: mdl-36385532

RESUMEN

A step towards the next generation of high-capacity, noise-resilient communication and computing technologies is a substantial increase in the dimensionality of information space and the synthesis of superposition states on an N-dimensional (N > 2) Hilbert space featuring exotic group symmetries. Despite the rapid development of photonic devices and systems, on-chip information technologies are mostly limited to two-level systems owing to the lack of sufficient reconfigurability to satisfy the stringent requirement for 2(N - 1) degrees of freedom, intrinsically associated with the increase of synthetic dimensionalities. Even with extensive efforts dedicated to recently emerged vector lasers and microcavities for the expansion of dimensionalities1-10, it still remains a challenge to actively tune the diversified, high-dimensional superposition states of light on demand. Here we demonstrate a hyperdimensional, spin-orbit microlaser for chip-scale flexible generation and manipulation of arbitrary four-level states. Two microcavities coupled through a non-Hermitian synthetic gauge field are designed to emit spin-orbit-coupled states of light with six degrees of freedom. The vectorial state of the emitted laser beam in free space can be mapped on a Bloch hypersphere defining an SU(4) symmetry, demonstrating dynamical generation and reconfiguration of high-dimensional superposition states with high fidelity.


Asunto(s)
Comunicación , Tecnología de la Información , Fotones , Tecnología
2.
Ear Hear ; 45(3): 648-657, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38196103

RESUMEN

OBJECTIVES: Current approaches for evaluating noise-induced hearing loss (NIHL), such as the International Standards Organization 1999 (ISO) 1999 prediction model, rely mainly on noise energy and exposure time, thus ignoring the intricate time-frequency characteristics of noise, which also play an important role in NIHL evaluation. In this study, an innovative NIHL prediction model based on temporal and spectral feature extraction using an asymmetric convolution algorithm is proposed. DESIGN: Personal data and individual occupational noise records from 2214 workers across 23 factories in Zhejiang Province, China, were used in this study. In addition to traditional metrics like noise energy and exposure duration, the importance of time-frequency features in NIHL assessment was also emphasized. To capture these features, operations such as random sampling, windowing, short-time Fourier transform, and splicing were performed to create time-frequency spectrograms from noise recordings. Two asymmetric convolution kernels then were used to extract these critical features. These features, combined with personal information (e.g., age, length of service) in various configurations, were used as model inputs. The optimal network structure was selected based on the area under the curve (AUC) from 10-fold cross-validation, alongside the Wilcoxon signed ranks test. The proposed model was compared with the support vector machine (SVM) and ISO 1999 models, and the superiority of the new approach was verified by ablation experiments. RESULTS: The proposed model had an AUC of 0.7768 ± 0.0223 (mean ± SD), outperforming both the SVM model (AUC: 0.7504 ± 0.0273) and the ISO 1999 model (AUC: 0.5094 ± 0.0071). Wilcoxon signed ranks tests confirmed the significant improvement of the proposed model ( p = 0.0025 compared with ISO 1999, and p = 0.00142 compared with SVM). CONCLUSIONS: This study introduced a new NIHL prediction method that provides deeper insights into industrial noise exposure data. The results demonstrated the superior performance of the new model over ISO 1999 and SVM models. By combining time-frequency features and personal information, the proposed approach bridged the gap between conventional noise assessment and machine learning-based methods, effectively improving the ability to protect workers' hearing.


Asunto(s)
Pérdida Auditiva Provocada por Ruido , Ruido en el Ambiente de Trabajo , Enfermedades Profesionales , Exposición Profesional , Humanos , Ruido en el Ambiente de Trabajo/efectos adversos , China
3.
Phys Rev Lett ; 131(18): 183801, 2023 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-37977645

RESUMEN

Quantum technologies, if scaled into a high-dimensional Hilbert space, can dramatically enhance connection capabilities with supporting higher bit rates and ultrasecure information transfer. Twisted single photons, carrying orbital angular momentum (OAM) as an unbounded dimension, could address the growing demand for high-dimensional quantum information encoding and transmission. By hybrid integration of two-dimensional semiconductor WSe_{2} with a spin-orbit-coupled microring resonator, we demonstrate an integrated tunable twisted single photon source with the ability to precisely define and switch between highly pure spin-OAM states. Our results feature a single photon purity of g^{(2)}(0)∼0.13 with a cavity-enhanced quantum yield of 76% and a high OAM mode purity up to 96.9%. Moreover, the demonstrated quantum-chiral control can also enable new quantum functionality such as single photon routing for efficient quantum information processing on chip.

4.
Environ Sci Technol ; 57(36): 13429-13438, 2023 09 12.
Artículo en Inglés | MEDLINE | ID: mdl-37642336

RESUMEN

The rubber antioxidant 6PPD has gained significant attention due to its highly toxic transformation product, 6PPD-quinone (6PPDQ). Despite their detection in urines of pregnant women, the placental transfer and developmental toxicity of 6PPD and 6PPDQ are unknown. Here, we treated C57Bl/6 mice with 4 mg/kg 6PPD or 6PPDQ to investigate their urine excretion and placental transfer. Female and male mice exhibited sex difference in excretion profiles of 6PPD and 6PPDQ. Urine concentrations of 6PPDQ were one order of magnitude lower than those of 6PPD, suggesting lower excretion and higher bioaccumulation of 6PPDQ. In pregnant mice treated with 6PPD or 6PPDQ from embryonic day 11.5 to 15.5, 6PPDQ showed ∼1.5-8 times higher concentrations than 6PPD in placenta, embryo body, and embryo brain, suggesting higher placental transfer of 6PPDQ. Using in vitro dual-luciferase reporter assays, we revealed that 6PPDQ activated the human retinoic acid receptor α (RARα) and retinoid X receptor α (RXRα) at concentrations as low as 0.3 µM, which was ∼10-fold higher than the concentrations detected in human urines. 6PPD activated the RXRα at concentrations as low as 1.2 µM. These results demonstrate the exposure risks of 6PPD and 6PPDQ during pregnancy and emphasize the need for further toxicological and epidemiological investigations.


Asunto(s)
Benzoquinonas , Desarrollo Embrionario , Fenilendiaminas , Animales , Femenino , Humanos , Masculino , Ratones , Embarazo , Benzoquinonas/metabolismo , Benzoquinonas/toxicidad , Benzoquinonas/orina , Placenta/metabolismo , Fenilendiaminas/metabolismo , Fenilendiaminas/toxicidad , Fenilendiaminas/orina , Ratones Endogámicos C57BL , Distribución Tisular , Factores Sexuales , Desarrollo Embrionario/efectos de los fármacos , Células HEK293 , Receptor alfa de Ácido Retinoico/metabolismo , Receptor alfa X Retinoide/metabolismo
5.
Environ Sci Technol ; 57(14): 5621-5632, 2023 04 11.
Artículo en Inglés | MEDLINE | ID: mdl-36996351

RESUMEN

6PPD, a tire rubber antioxidant, poses substantial ecological risks because it can form a highly toxic quinone transformation product (TP), 6PPD-quinone (6PPDQ), during exposure to gas-phase ozone. Important data gaps exist regarding the structures, reaction mechanisms, and environmental occurrence of TPs from 6PPD ozonation. To address these data gaps, gas-phase ozonation of 6PPD was conducted over 24-168 h and ozonation TPs were characterized using high-resolution mass spectrometry. The probable structures were proposed for 23 TPs with 5 subsequently standard-verified. Consistent with prior findings, 6PPDQ (C18H22N2O2) was one of the major TPs in 6PPD ozonation (∼1 to 19% yield). Notably, 6PPDQ was not observed during ozonation of 6QDI (N-(1,3-dimethylbutyl)-N'-phenyl-p-quinonediimine), indicating that 6PPDQ formation does not proceed through 6QDI or associated 6QDI TPs. Other major 6PPD TPs included multiple C18H22N2O and C18H22N2O2 isomers, with presumptive N-oxide, N,N'-dioxide, and orthoquinone structures. Standard-verified TPs were quantified in roadway-impacted environmental samples, with total concentrations of 130 ± 3.2 µg/g in methanol extracts of tire tread wear particles (TWPs), 34 ± 4 µg/g-TWP in aqueous TWP leachates, 2700 ± 1500 ng/L in roadway runoff, and 1900 ± 1200 ng/L in roadway-impacted creeks. These data demonstrate that 6PPD TPs are likely an important and ubiquitous class of contaminants in roadway-impacted environments.


Asunto(s)
Antioxidantes , Benzoquinonas , Fenilendiaminas , Goma , Antioxidantes/química , Ozono/química , Goma/química , Agua/química , Fenilendiaminas/química , Benzoquinonas/química
6.
Environ Sci Technol ; 57(7): 2779-2791, 2023 02 21.
Artículo en Inglés | MEDLINE | ID: mdl-36758188

RESUMEN

Recently, roadway releases of N,N'-substituted p-phenylenediamine (PPD) antioxidants and their transformation products (TPs) received significant attention due to the highly toxic 6PPD-quinone. However, the occurrence of PPDs and TPs in recycled tire rubber products remains uncharacterized. Here, we analyzed tire wear particles (TWPs), recycled rubber doormats, and turf-field crumb rubbers for seven PPD antioxidants, five PPD-quinones (PPDQs), and five other 6PPD TPs using liquid chromatography-tandem mass spectrometry. PPD antioxidants, PPDQs, and other TPs were present in all samples with chemical profiles dominated by 6PPD, DTPD, DPPD, and their corresponding PPDQs. Interestingly, the individual [PPDQ]/[PPD] and [TP]/[PPD] ratios significantly increased as total concentrations of the PPD-derived chemical decreased, indicating that TPs (including PPDQs) dominated the PPD-derived compounds with increased environmental weathering. Furthermore, we quantified 15 other industrial rubber additives (including bonding agents, vulcanization accelerators, benzotriazole and benzothiazole derivatives, and diphenylamine antioxidants), observing that PPD-derived chemical concentrations were 0.5-6 times higher than these often-studied additives. We also screened various other elastomeric consumer products, consistently detecting PPD-derived compounds in lab stoppers, sneaker soles, and rubber garden hose samples. These data emphasize that PPD antioxidants, PPDQs, and related TPs are important, previously overlooked contaminant classes in tire rubbers and elastomeric consumer products.


Asunto(s)
Antioxidantes , Benzoquinonas , Fenilendiaminas , Goma , Antioxidantes/análisis , Antioxidantes/química , Antioxidantes/clasificación , Fenilendiaminas/análisis , Fenilendiaminas/química , Fenilendiaminas/clasificación , Goma/química , Benzoquinonas/análisis , Benzoquinonas/química , Benzoquinonas/clasificación , Cromatografía Líquida con Espectrometría de Masas , Espectrometría de Masas en Tándem
7.
J Transl Med ; 19(1): 295, 2021 07 08.
Artículo en Inglés | MEDLINE | ID: mdl-34238315

RESUMEN

BACKGROUND: Metastasis and invasion are crucial in determining the mortality of cervical carcinoma (CC) patients. The epithelial-mesenchymal transition (EMT) is now a universal explanation for the mechanisms of tumor metastasis. Α-chimeric protein (α-chimaerin, CHN1) plays an important role in the regulation of signal transduction and development. However, the molecular regulatory relationships between CHN1 and CC progression in relation to EMT have not yet been identified. METHODS: The expression of CHN1 in CC tissues, adjacent tissues, and lymph node metastases from CC patients was detected by immunohistochemistry. Upregulation and knockdown of CHN1 were achieved by transfection of CC cells. The effect of CHN1 on cell proliferation was determined by CCK-8 and plate clone formation assays. Changes in migration and invasion capabilities were evaluated using scratch migration and transwell invasion assays. The effect of CHN1 overexpression and interference on xenograft tumor growth was determined by tumor weight and pathological analyses. The expression of EMT-related mRNAs was measured by qRT-PCR in transfected CC cells. EMT-related proteins and Akt/GSK-3ß/Snail signaling pathway-related proteins were also evaluated by western blotting. RESULTS: CHN1 was overexpressed in CC tissues and was associated with lymph node metastasis and low survival in CC patients. Overexpression of CHN1 promoted cell proliferation, migration, and invasion in CC cells. In contrast, silencing of CHN1 inhibited these phenomena. Overexpression of CHN1 promoted tumor formation in an in vivo xenograft tumor mouse model, with increased tumor volumes and weights. In addition, CHN1 induced the expression of EMT-related transcription factors, accompanied by the decreased expression of epithelial markers and increased expression of mesenchymal markers. The Akt/GSK-3ß/Snail signaling pathway was activated by overexpression of CHN1 in vitro, and activation of this pathway was inhibited by the signaling pathway inhibitor LY294002. CONCLUSION: These results suggest that CHN1 promotes the development and progression of cervical carcinoma via the Akt/GSK-3ß/Snail pathway by inducing EMT.


Asunto(s)
Carcinoma , Transición Epitelial-Mesenquimal , Animales , Línea Celular Tumoral , Movimiento Celular , Proliferación Celular , Quimerina 1 , Regulación Neoplásica de la Expresión Génica , Glucógeno Sintasa Quinasa 3 beta , Humanos , Ratones , Proteínas Proto-Oncogénicas c-akt/metabolismo , Factores de Transcripción de la Familia Snail/genética , Factores de Transcripción de la Familia Snail/metabolismo
8.
Environ Sci Technol ; 55(5): 3070-3080, 2021 03 02.
Artículo en Inglés | MEDLINE | ID: mdl-33600148

RESUMEN

Current aquatic toxicity assessments usually focus on targeted analyses coupled with toxicity testing to determine the impacts of complex mixtures on aquatic organisms. However, based on this approach alone, it is sometimes difficult to explain observed toxicity from the selected chemical analytes. Recent analytical advances such as high-resolution mass spectrometry (HRMS) can improve the characterizations of the chemical composition of complex mixtures, but the intensive labor required to produce confident identifications limits its utility in high-throughput screening. In the present study, we evaluated a rapid workflow to predict potential toxicity signatures of complex water samples based on high-throughput, tentative HRMS identifications derived from database matching, followed by identification of chemical-ligand interactions and pathway identification. We tested the workflow with water samples from the effluent-dominated Lubbock Canyon Lake System (LCLS). Results across all sites showed that predicted toxicity signatures had little variation when correcting for HRMS false-positive rates. The most common pathways across sites were gonadotropin-releasing hormone receptor and α-adrenergic receptor signaling. Alterations to the predicted pathways were successfully observed in larval zebrafish exposures to LCLS water samples. These results may allow researchers to better utilize rapid assessments of HRMS data for the assessment of adverse impacts on aquatic organisms.


Asunto(s)
Ríos , Contaminantes Químicos del Agua , Animales , Lagos , Espectrometría de Masas , Contaminantes Químicos del Agua/análisis , Contaminantes Químicos del Agua/toxicidad , Pez Cebra
9.
Environ Sci Technol ; 55(20): 13869-13880, 2021 10 19.
Artículo en Inglés | MEDLINE | ID: mdl-34582191

RESUMEN

Dienogest (DIE) and drospirenone (DRO) are two fourth-generation synthetic progestins widely used as oral contraceptives. Despite their increasing detection in wastewaters and surface waters, their fate during biological wastewater treatment is unclear. Here, we investigated DIE and DRO biotransformation with representative activated sludge batch incubations and identified relevant transformation products (TPs) using high-resolution mass spectrometry. DIE exhibited slow biotransformation (16-30 h half-life) and proceeded through a quantitative aromatic dehydrogenation to form TP 309 (molar yields of ∼55%), an aromatic TP ∼30% estrogenic as 17ß-estradiol. DRO experienced more rapid biotransformation (<0.5 h half-life), and 1,2-dehydrogenation formed the major TP 364 (molar yields of ∼40%), an antimineralocorticoid drug candidate named as spirorenone. Lactone ring hydrolysis was another important biotransformation pathway for DRO (molar yields of ∼20%) and generated pharmacologically inactive TP 384. Other minor pathways for DIE and DRO included hydroxylation, methoxylation, and 3-keto and C4(5) double-bond hydrogenation; distinct bioactivities are plausible for such TPs, including antigestagenic activity, antigonadotropic activity, and pregnancy inhibition effects. Thus, biotransformation products of DIE and DRO during wastewater treatment should be considered in environmental assessments of synthetic progestins, especially certain TPs such as the estrogenic TP 309 of DIE and the antimineralocorticoid spirorenone (TP 364) of DRO.


Asunto(s)
Progestinas , Aguas del Alcantarillado , Androstenos , Biotransformación , Femenino , Humanos , Laboratorios , Nandrolona/análogos & derivados , Embarazo
10.
BMC Cancer ; 20(1): 1029, 2020 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-33109127

RESUMEN

BACKGROUND: Cervical cancer is the leading cause of cancer-related death in women worldwide. However, the mechanisms mediating the development and progression of cervical cancer are unclear. In this study, we aimed to elucidate the roles of microRNAs and a1-chimaerin (CHN1) protein in cervical cancer progression. METHODS: The expression of miR-205 and CHN1 protein was investigated by in situ hybridisation and immunohistochemistry. We predicted the target genes of miR-205 using software prediction and dual luciferase assays. The expression of mRNAs and proteins was tested by qRT-PCR and western blotting respectively. The ability of cell growth, migration and invasion was evaluated by CCK-8 and transwell. Cell apoptosis was analysed by flow cytometry analysis. RESULTS: We found that miR-205 and CHN1 were highly expressed in human cervical cancer tissue compared with paired normal cervical tissues. The CHN1 gene was shown to be targeted by miR-205 in HeLa cells. Interestingly, transfection with miR-205 mimic upregulated CHN1 mRNA and protein, while miR-205 inhibitor downregulated CHN1 in high-risk and human papilloma virus (HPV)-negative human cervical cancer cells in vitro,. These data suggested that miR-205 positively regulated the expression of CHN1. Furthermore, the miR-205 mimic promoted cell growth, apoptosis, migration, and invasion in high-risk and HPV-negative cervical cancer cells, while the miR-205 inhibitor blocked these biological processes. Knockdown of CHN1 obviously reduced the aggressive cellular behaviours induced by upregulation of miR-205, suggesting that miR-205 positively regulated CHN1 to mediate these cell behaviours during the development of cervical cancer. Furthermore, CHN1 was correlated with lymph node metastasis in clinical specimens. CONCLUSIONS: Our findings showed that miR-205 positively regulated CHN1 to mediate cell growth, apoptosis, migration, and invasion during cervical cancer development, particularly for high-risk HPV-type cervical cancer. These findings suggested that dysregulation of miR-205 and subsequent abnormalities in CHN1 expression promoted the oncogenic potential of human cervical cancer.


Asunto(s)
Quimerina 1/genética , Metástasis Linfática/genética , MicroARNs/genética , Regulación hacia Arriba , Neoplasias del Cuello Uterino/genética , Línea Celular Tumoral , Movimiento Celular , Proliferación Celular , Quimerina 1/metabolismo , Femenino , Regulación Neoplásica de la Expresión Génica , Técnicas de Silenciamiento del Gen , Células HeLa , Humanos , Neoplasias del Cuello Uterino/metabolismo
11.
Environ Sci Technol ; 54(2): 889-901, 2020 01 21.
Artículo en Inglés | MEDLINE | ID: mdl-31887037

RESUMEN

This study used suspect and nontarget screening with high-resolution mass spectrometry to characterize the occurrence of contaminants of emerging concern (CECs) in the nearshore marine environment of Puget Sound (WA). In total, 87 non-polymeric CECs were identified; those confirmed with reference standards (45) included pharmaceuticals, herbicides, vehicle-related compounds, plasticizers, and flame retardants. Eight polyfluoroalkyl substances were detected; perfluorooctanesulfonic acid (PFOS) concentrations were as high as 72-140 ng/L at one location. Low levels of methamphetamine were detected in 41% of the samples. Transformation products of pesticides were tentatively identified, including two novel transformation products of tebuthiuron. While a hydrodynamic simulation, analytical results, and dilution calculations demonstrated the prevalence of wastewater effluent to nearshore marine environments, the identity and abundance of selected CECs revealed the additional contributions from stormwater and localized urban and industrial sources. For the confirmed CECs, risk quotients were calculated based on concentrations and predicted toxicities, and eight CECs had risk quotients >1. Dilution in the marine estuarine environment lowered the risks of most wastewater-derived CECs, but dilution alone is insufficient to mitigate risks of localized inputs. These findings highlighted the necessity of suspect and nontarget screening and revealed the importance of localized contamination sources in urban marine environments.


Asunto(s)
Retardadores de Llama , Contaminantes Químicos del Agua , Monitoreo del Ambiente , Estuarios , Aguas Residuales
12.
Reproduction ; 157(2): 149-161, 2019 02 01.
Artículo en Inglés | MEDLINE | ID: mdl-30601756

RESUMEN

Stress impacts the reproductive axis at the level of the hypothalamus and the pituitary gland, which exert an effect on the ovary. Menstruation is regulated by the hypothalamic-pituitary-ovary (HPO) axis. However, the role of stress in menstruation remains unclear. The objective of this study was to explore the role of stress in endometrial breakdown and shedding, using the pseudopregnant mouse menstrual-like model. Female mice were mated with vasectomized males and labeled day 0.5, upon observation of a vaginal seminal plug. On day 3.5, decidualization was induced in pseudopregnant mice using arachis oil. On day 5.5, pseudopregnant mice with artificial decidualization were placed in restraint tubes for 3 h. The findings indicated that acute restraint stress resulted in the disintegration of the endometrium. While corticosterone concentration in the serum increased significantly due to restraint stress, follicle-stimulating hormone (FSH), luteinizing hormone (LH) and progesterone (P4) levels in the serum decreased significantly. An endometrial histology examination indicated that progesterone implants may rescue P4 decline caused by acute stress and block endometrium breakdown and shedding. In addition, mice were treated with metyrapone, an inhibitor of corticosterone synthesis, 1 h prior to being subjected to restraint stress. Interestingly, metyrapone not only inhibited stress-induced endometrium breakdown and shedding, but also prevented stress-induced reduction of P4, LH and FSH. Furthermore, real-time PCR and western blot showed that mRNA and protein expression of CYP11A1 (cytochrome P450, family 11, subfamily A, polypeptide 1) and steroidogenic acute regulatory protein (StAR), the two rate-limiting enzymes for progesterone synthesis in the ovary, decreased following acute stress. But metyrapone prevented the reduction of StAR expression induced by restraint stress. Overall, this study revealed that acute stress results in an increase in corticosterone, which may inhibit LH and FSH release in the serum and CYP11A1 and StAR expression in the ovary, which finally leads to the breakdown and shedding of the endometrium. These experimental findings, based on the mouse model, may enable further understanding of the effects of stress on menstruation regulation and determine the potential factors affecting stress-associated menstrual disorders.


Asunto(s)
Corticosterona/sangre , Endometrio/patología , Progesterona/sangre , Estrés Fisiológico/fisiología , Estrés Psicológico/patología , Animales , Endometrio/efectos de los fármacos , Inhibidores Enzimáticos/farmacología , Femenino , Hormona Folículo Estimulante/sangre , Hormona Luteinizante/sangre , Metirapona/farmacología , Ratones , Progesterona/farmacología , Restricción Física
13.
Anal Bioanal Chem ; 411(29): 7791-7806, 2019 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-31701207

RESUMEN

Pollutants transported in urban stormwater runoff induce pervasive water quality degradation in receiving waters. To accurately characterize stormwater quality and treatment system performance across the range of possible contaminant characteristics, comprehensive multi-residue analytical methods are necessary. Here, we developed a solid-phase extraction (SPE) and high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) method to quantify representative stormwater-derived organic contaminants across multiple chemical classes, including vehicle-related chemicals, corrosion inhibitors, industrial chemicals, pesticides, pharmaceuticals and personal care products, and antioxidants. Extraction conditions, isotope-labeled internal standards, and LC-MS/MS parameters were optimized to enhance recovery, minimize matrix effects, and maximize selectivity and sensitivity. The developed method was sensitive (method quantification limits < 10 ng/L for > 80% of selected analytes) and accurate (mean relative recoveries in the range of 70-130%, with relative standard deviations < 25% for 77% of the analytes) for most of the analytes. The method was used to analyze samples collected from nine urban watersheds during a storm event; 62% of the 39 analytes were detected at least once at concentrations up to 540 ng/L (1,3-diphenylguanidine). Spatial trends in detection and concentration were observed for vehicle-related and industrial chemicals that correlated with vehicle traffic. Total concentrations of pesticides suggested that residential uses could be more important sources than agriculture. This study illustrates the pervasive occurrence of a wide variety of stormwater-derived chemicals in urban receiving waters and highlights the need to better understand their environmental fate and ecological implications. Graphical abstract.

14.
Environ Sci Technol ; 52(8): 4632-4640, 2018 04 17.
Artículo en Inglés | MEDLINE | ID: mdl-29608280

RESUMEN

Despite the increasing use and discharge of novel brominated flame retardants, little information is available about their trophodynamics in the aquatic food web, and their subsequent relationships to compound metabolism. In this study, concentrations of 2,4,6-tribromophenyl allyl ether (ATE), 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH), tetrabromo- o-chlorotoluene (TBCT), pentabromobenzyl acrylate (PBBA), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), bis(2-ethylhexyl)-3,4,5,6-tetrabromo-phthalate (TBPH), and decabromodiphenyl ethane (DBDPE) were measured in 17 species, including plankton, invertebrates, and fish from Lake Taihu, South China. Trophodynamics of the compounds were assessed, and metabolic rates were measured in the liver microsomes of crucian (trophic level [TL]: 2.93), catfish (TL: 3.86), and yellow-head catfish (TL: 4.3). Significantly positive relationships were found between trophic levels and lipid-normalized concentrations of ATE, BTBPE, and TBPH; their trophic magnification factors (TMFs) were 2.85, 2.83, and 2.42, respectively. Consistently, the three chemicals were resistant to metabolism in all fish microsomes. No significant relationship was observed for ßTBECH ( p = 0.116), and DBDPE underwent trophic dilution in the food web (TMFs = 0.37, p = 0.021). Moreover, these two chemicals showed steady metabolism with incubation time in all fish microsomes. TBCT and PBBA exhibited significant trophic magnifications in the food web (TMF = 4.56, 2.01). Though different metabolic rates were observed for the two compounds among the tested fish species, TBCT and PBBA both showed metabolic resistance in high-trophic-level fish. These results indicated that metabolism of organisms at high trophic levels plays an important role in the assessment of trophic magnification potentials of these flame retardant chemicals.


Asunto(s)
Retardadores de Llama , Hidrocarburos Bromados , Contaminantes Químicos del Agua , Animales , China , Monitoreo del Ambiente , Peces , Cadena Alimentaria , Éteres Difenilos Halogenados , Lagos
16.
Environ Sci Technol ; 50(16): 8896-903, 2016 08 16.
Artículo en Inglés | MEDLINE | ID: mdl-27434659

RESUMEN

While a recent toxicological study has shown that organophosphorus flame retardants (OPFRs) may disrupt sphingolipid homeostasis, epidemiologic evidence is currently lacking. In this study, a total of 257 participants were recruited from Shenzhen, China. Eleven OPFRs were for the first time simultaneously determined in the human blood samples by ultraperformance liquid chromatography and tandem mass spectrometry. Six OPFRs, tributyl phosphate (TNBP), 2-ethylhexyl diphenyl phosphate (EHDPP), tris(2-chloroisopropyl) phosphate (TCIPP), tris(2-butoxyethyl) phosphate (TBOEP), triethyl phosphate (TEP), and TPHP, were detectable in at least 90% of participants, with median concentrations of 37.8, 1.22, 0.71, 0.54, 0.49, and 0.43 ng/mL, respectively. Sphingomyelin (SM) levels in the highest quartile of EHDPP, TPHP, TNBP, TBOEP, TEP, and TCIPP were 45.3% [95% confidence interval; 38.1%, 53.0%], 51.9% (45.5%, 58.6%), 153.6% (145.1%, 162.3%), 20.6% (14.5%, 27.0%), 59.0% (52.1%, 66.2%), and 62.8% (55.2%, 70.6%) higher than those in the lowest quartile, respectively, after adjusting for covariates. Sphingosine 1-phosphate (S1P) levels in the highest quartile of EHDPP, TPHP, and TNBP were 36% (-39%, -33%), 16% (-19%, -14%), and 36% (-38%, -33%) lower than those in the lowest quartile, respectively. A similar pattern emerged when exposures were modeled continuously. We for the first time found the associations between OPFRs and changes in human sphingolipid homeostasis.


Asunto(s)
Retardadores de Llama , Compuestos Organofosforados , China , Homeostasis , Humanos , Esfingolípidos
17.
mSystems ; 9(3): e0111923, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38319107

RESUMEN

Skin microbiome can be altered in patients with atopic dermatitis (AD). An understanding of the changes from healthy to atopic skin can help develop new targets for treatment by identifying microbial and molecular biomarkers. This study investigates the skin microbiome and metabolome of healthy adult subjects and lesion (ADL) and non-lesion (ADNL) of AD patients by 16S rRNA gene sequencing and mass spectrometry, respectively. Samples from AD patients showed alterations in the diversity and composition of the skin microbiome, with ADL skin having the greatest divergence. Staphylococcus species, especially S. aureus, were significantly increased in AD patients. Metabolomic profiles were also different between the groups. Dipeptide derivatives are more abundant in ADL, which may be related to skin inflammation. Co-occurrence network analysis of the microbiome and metabolomics data revealed higher co-occurrence of metabolites and bacteria in healthy ADNL compared to ADL. S. aureus co-occurred with dipeptide derivatives in ADL, while phytosphingosine-derived compounds showed co-occurrences with commensal bacteria, for example, Paracoccus sp., Pseudomonas sp., Prevotella bivia, Lactobacillus iners, Anaerococcus sp., Micrococcus sp., Corynebacterium ureicelerivorans, Corynebacterium massiliense, Streptococcus thermophilus, and Roseomonas mucosa, in healthy and ADNL groups. Therefore, these findings provide valuable insights into how AD affects the human skin metabolome and microbiome.IMPORTANCEThis study provides valuable insight into changes in the skin microbiome and associated metabolomic profiles in an adult population with mild to moderate atopic dermatitis. It also identifies new therapeutic targets that may be useful for developing personalized treatments for individuals with atopic dermatitis based on their unique skin microbiome and metabolic profiles.


Asunto(s)
Dermatitis Atópica , Microbiota , Adulto , Humanos , Dermatitis Atópica/tratamiento farmacológico , Staphylococcus aureus/genética , ARN Ribosómico 16S/genética , Microbiota/genética , Metaboloma , Bacterias/genética , Dipéptidos/uso terapéutico
18.
bioRxiv ; 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38798440

RESUMEN

Understanding the distribution of hundreds of thousands of plant metabolites across the plant kingdom presents a challenge. To address this, we curated publicly available LC-MS/MS data from 19,075 plant extracts and developed the plantMASST reference database encompassing 246 botanical families, 1,469 genera, and 2,793 species. This taxonomically focused database facilitates the exploration of plant-derived molecules using tandem mass spectrometry (MS/MS) spectra. This tool will aid in drug discovery, biosynthesis, (chemo)taxonomy, and the evolutionary ecology of herbivore interactions.

19.
Environ Sci Process Impacts ; 25(5): 901-911, 2023 May 25.
Artículo en Inglés | MEDLINE | ID: mdl-37042393

RESUMEN

We here report chemical characteristics relevant to the fate and transport of the recently discovered environmental toxicant 6PPD-quinone (2-((4-methylpentan-2-yl)amino)-5-(phenylamino)cyclohexa-2,5-diene-1,4-dione or "6PPDQ"). 6PPDQ is a transformation product of the tire rubber antioxidant 6PPD that is ubiquitous in roadway environments, including atmospheric particulate matter, soils, runoff, and receiving waters, after dispersal from tire rubber use and wear on roadways. The aqueous solubility and octanol-water partitioning coefficient (i.e. log KOW) for 6PPDQ were measured to be 38 ± 10 µg L-1 and 4.30 ± 0.02, respectively. Within the context of analytical measurement and laboratory processing, sorption to various laboratory materials was evaluated, indicating that glass was largely inert but loss of 6PPDQ to other materials was common. Aqueous leaching simulations from tire tread wear particles (TWPs) indicated short term release of ∼5.2 µg 6PPDQ per gram TWP over 6 h under flow-through conditions. Aqueous stability tests observed a slight-to-moderate loss of 6PPDQ over 47 days (26 ± 3% loss) for pH 5, 7 and 9. These measured physicochemical properties suggest that 6PPDQ is generally poorly soluble but fairly stable over short time periods in simple aqueous systems. 6PPDQ can also leach readily from TWPs for subsequent environmental transport, posing high potential for adverse effects in local aquatic environments.


Asunto(s)
Benzoquinonas , Sustancias Peligrosas , Fenilendiaminas , Goma , Contaminantes Químicos del Agua , Sustancias Peligrosas/química , Material Particulado/química , Agua/química , Contaminantes Químicos del Agua/química , Fenilendiaminas/química , Benzoquinonas/química , Solubilidad
20.
Nat Commun ; 14(1): 3206, 2023 Jun 02.
Artículo en Inglés | MEDLINE | ID: mdl-37268611

RESUMEN

Graphene, with its two linearly dispersing Dirac points with opposite windings, is the minimal topological nodal configuration in the hexagonal Brillouin zone. Topological semimetals with higher-order nodes beyond the Dirac points have recently attracted considerable interest due to their rich chiral physics and their potential for the design of next-generation integrated devices. Here we report the experimental realization of the topological semimetal with quadratic nodes in a photonic microring lattice. Our structure hosts a robust second-order node at the center of the Brillouin zone and two Dirac points at the Brillouin zone boundary-the second minimal configuration, next to graphene, that satisfies the Nielsen-Ninomiya theorem. The symmetry-protected quadratic nodal point, together with the Dirac points, leads to the coexistence of massive and massless components in a hybrid chiral particle. This gives rise to unique transport properties, which we demonstrate by directly imaging simultaneous Klein and anti-Klein tunnelling in the microring lattice.

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