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•6:2 Cl-PFAES and TFA are detected with high levels in serum, second to PFOA and PFOS.•A significant increase in 6:2 Cl-PFAES with age and BMI, and TFA with age are found.•Positive ...associations of several PFASs with fasting glucose and HbA1c are observed.
In recent years, the occurrence of novel per-/polyfluoroalkyl substances (PFASs) such as polyfluoroalkyl ether sulfonates (PFAESs) in human samples have aroused attention due to the change in PFASs production profile, however, the data are still lacking. Furthermore, epidemiological studies have examined the associations of PFAS exposure with glucose homeostasis, but with inconsistent results. Therefore, in this study, fasting serum samples from 252 participants with an age range from 19 to 87 years old were collected in Tianjin, China. A total of 21 target PFASs were determined to analyze the levels and distribution of novel and legacy PFASs in serum and to further evaluate the cross-sectional associations of serum PFAS concentrations with two glycemic biomarkers (i.e., fasting glucose and glycated hemoglobin (HbA1c)). 6:2 chlorinated PFAES (6:2 Cl-PFAES) and trifluoroacetic acid (TFA) were widely detected novel PFASs (greater than90%) with relatively high median concentrations (8.64 ng/mL and 8.46 ng/mL, respectively), which were second only to the two dominant legacy PFASs, i.e., perfluorooctanoic acid (PFOA, 14.83 ng/mL) and perfluorooctane sulfonic acid (14.24 ng/mL). The percentage contributions to the total known PFASs were separately 17.6% and 17.2% for 6:2 Cl-PFAES and TFA. The levels of 6:2 Cl-PFAES were significantly correlated with age and BMI, and the concentrations of TFA were also significantly correlated with age. Furthermore, 1% increase in serum PFOA and perfluorononanoic acid (PFNA) was separately significantly associated with 0.018% 95% confidence interval (CI): 0.004%, 0.033% and 0.022% (95% CI: 0.007%, 0.037%) increment in fasting glucose levels. Similarly, 1% increase in serum perfluorohexanoic acid, PFNA, and perfluorohexane sulfonic acid was significantly associated with 0.030% (95% CI: 0.010%, 0.051%), 0.018% (95% CI: 0.003%, 0.033%), 0.007% (95% CI: 0.003%, 0.011%) increment in HbA1c levels, respectively. These findings suggested that 6:2 Cl-PFAES and TFA showed greater contributions to PFASs in serum and supported an association of exposure to PFASs with fasting glucose and HbA1c.
Developing low-cost, high-performance electrocatalysts for the hydrogen evolution reaction (HER) is essential for producing hydrogen from renewable energy sources. Herein, we report phosphated IrMo ...bimetallic clusters supported by macroporous nitrogen-doped carbon (IrMoP/MNC) as a highly efficient alkaline HER catalyst. The experimental and theoretical results demonstrate that P and Mo synergistically tune the electronic structure of atomically dispersed Ir to improve adsorption of the reactant H2O and desorption of the product OH−. P itself serves as an active site and cooperates with the nearby Ir atom to significantly enhance the HER kinetics. Even with only 2.6 wt% Ir in the catalyst, IrMoP/MNC exhibits an ultralow overpotential of 14 mV at 10 mA cm−2, as well as an unprecedented high mass activity of 18.58 A mgIr−1 at an overpotential of 100 mV, superior to commercial Pt/C and overwhelmingly better than other Ir-based electrocatalysts. This study demonstrates a multi-level design strategy to effectively improve the atom efficiency of a noble metal, involving spatial geometry, local electronic structure, and dual-atom synergy.
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•Phosphated IrMo clusters with high noble metal utilization are synthesized as an electrocatalyst for the alkaline hydrogen evolution reaction.•Phosphorus optimizes the electronic structure of Ir and synergistically decomposes water molecules with Ir to enhance the HER kinetics.•Macroporous carbon-supported IrMoP clusters exhibit an ultralow overpotential and high mass activity for the alkaline HER.
Iron-based Prussian blue analogs are promising low-cost and easily prepared cathode materials for sodium-ion batteries. Their materials quality and electrochemical performance are heavily reliant on ...the precipitation process. Here we report a controllable precipitation method to synthesize high-performance Prussian blue for sodium-ion storage. Characterization of the nucleation and evolution processes of the highly crystalline Prussian blue microcubes reveals a rhombohedral structure that exhibits high initial Coulombic efficiency, excellent rate performance, and cycling properties. The phase transitions in the as-obtained material are investigated by synchrotron in situ powder X-ray diffraction, which shows highly reversible structural transformations between rhombohedral, cubic, and tetragonal structures upon sodium-ion (de)intercalations. Moreover, the Prussian blue material from a large-scale synthesis process shows stable cycling performance in a pouch full cell over 1000 times. We believe that this work could pave the way for the real application of Prussian blue materials in sodium-ion batteries.
Non-precious-metal or metal-free catalysts with stability are desirable but challenging for proton exchange membrane fuel cells. Here we partially unzip a multiwall carbon nanotube to synthesize ...zigzag-edged graphene nanoribbons with a carbon nanotube backbone for electrocatalysis of oxygen reduction in proton exchange membrane fuel cells. Zigzag carbon exhibits a peak areal power density of 0.161 W cm
and a peak mass power density of 520 W g
, superior to most non-precious-metal electrocatalysts. Notably, the stability of zigzag carbon is improved in comparison with a representative iron-nitrogen-carbon catalyst in a fuel cell with hydrogen/oxygen gases at 0.5 V. Density functional theory calculation coupled with experimentation reveal that a zigzag carbon atom is the most active site for oxygen reduction among several types of carbon defects on graphene nanoribbons in acid electrolyte. This work demonstrates that zigzag carbon is a promising electrocatalyst for low-cost and durable proton exchange membrane fuel cells.
•OPE metabolites were investigated in urine samples of pregnant women (n = 360).•OPE metabolites were positively associated with maternal and neonatal TSH.•Associations between OPE metabolites and ...thyroid hormones differed by newborn sex.•OPE metabolites were positively associated with maternal urinary 8-OhdG and MDA.•8-OhdG highly mediates (63.1%) the association between DPHP and neonatal TSH.
Organophosphate esters (OPEs) are widely used as flame retardants and plasticizers in consumer and industrial products. Human exposure to OPEs raises concerns due to their endocrine disruptive potentials. Till now, the effects of OPEs on thyroid hormones (THs) and the mediating role of oxidative stress in pregnant women have not been studied. In this study, prenatal urinary concentrations of OPE metabolites (mOPEs), levels of free triiodothyronine (FT3), free thyroxine (FT4), thyroid-stimulating hormone (TSH), and oxidative stress levels of 8-hydroxy-2-deoxy guanosine (8-OHdG) and malondialdehyde (MDA) were measured in pregnant women (n = 360) from a coastal urbanized region and moderate socioeconomic status. Neonatal TSH in heel blood was also measured in newborns (n = 309). Dibutyl phosphate (DBP) and diphenyl phosphate (DPHP) were extensively detected with a median creatinine-adjusted level of 0.19 μg/g and 0.66 μg/g, respectively, and the median of ∑mOPEs was 1.82 μg/g. DBP and DPHP were included in the analysis. The concentrations of DBP and DPHP were positively associated with either maternal or neonatal TSH levels, while not for maternal FT3 and FT4 levels. Positive associations for maternal and neonatal TSH were particularly observed in girls as stratified by newborn sex suggesting a sex-selective difference. Furthermore, 8-OHdG, the biomarker of DNA damage, was found to be a major mediator (>60%) for the association between neonatal TSH and DPHP, suggesting that DNA damage is involved in fetal thyroid function disruption. On the other hand, MDA showed a partially suppressing effect (<40%) for the associations between mOPEs and neonatal TSH, which needs further clarification. For maternal TSH, both 8-OHdG and MDA showed moderate mediating effects while the direct effects of mOPEs on maternal TSH also contributed. These results suggest thyroid disrupting effects of OPE exposure on mothers and fetuses during pregnancy and the potential influence mediated by the oxidative stresses of DNA damage and lipid peroxidation.
The objective of this study is to explore the effect and mechanism of ultrasound on chitin extraction from shrimp shells powder (SSP) by the co-fermentation of Bacillus subtilis and Acetobacter ...pasteurianus. After pre-treating the SSP with high-intensity ultrasound (HIU) at 800 W, the protease activity in the fermentation solution reached 96.9 U/mL on day 3, which was significantly higher than for SSP that had not been pre-treated with ultrasound (81.8 U/mL). The fermentation time of the chitin extraction process was 5.0 d without ultrasound pre-treatment, while it was shortened to 4.5 d when using ultrasound at 800 W to treat SSP. However, there were no obvious differences when we applied ultrasound at low power (200 W, 400 W). Furthermore, chitin purified from shrimp shells pre-treated with HIU at 800 W exhibited lower molecular weight (11.2 kDa), higher chitin purity (89.8%), and a higher degree of deacetylation (21.1%) compared to SSP with no ultrasound pre-treatment (13.5 kDa, 86.6%, 18.5%). Results indicate that HIU peels off the protein/CaCO3 matrix that covers the SSP surface. About 9.1% of protein and 4.7% of Ca2+ were released from SSP pre-treated with HIU at 800 W. These figures were both higher than with no ultrasound pre-treatment (4.5%, 3.2%). Additionally, the amount of soluble protein extracted from SSP through HIU at 800 W was 50% higher than for the control sample. SDS-PAGE analysis indicated that the soluble protein was degraded to the micromolecule. It also revealed that HIU (600, 800 W) induced the secondary and tertiary structure destruction of protein extracted from SSP. In conclusion, HIU-induced degradation and structural damage of protein enhances the protein/CaCO3 matrix to be peeled off from SSP. Also, in the co-fermentation process, an increase of protease activity further accelerates deproteinization.
Elastic optical networks (EON) technology in combination with space division multiplexing (SDM) is considered as having the potential to expand the transmission capacity of optical transport ...networks. However, inter-core crosstalk may cause serious signal impairment in a multi-core fiber (MCF) links. At the same time, scheduled lightpath demands, for which the expected setup and teardown times are known in advance, are considered as an important type of traffic demand for future networks. In this article, we develop approaches to schedule simultaneous lightpaths onto non-adjacent MCF cores so as to reduce inter-core crosstalk between these lightpaths. To this end, we first define a new metric to estimate the inter-core crosstalk jointly considering the spatial, frequency, and time domains. We then tackle the routing, spectrum, core, and time assignment (RSCTA) problem for the MCF-based EON by developing an integer linear programming (ILP) model, as well as an auxiliary graph (AG) based heuristic algorithm, which jointly optimize spectrum resource utilization and reduce the lightpath inter-core crosstalk. Simulation studies show the effectiveness of the proposed approach in terms of both performance aspects. In addition, the performance of the proposed heuristic algorithm is shown to be close to that of the ILP model in small networks.
Effective and accurate diagnosis of Diabetes Mellitus (DM), as well as its early stage Impaired Glucose Regulation (IGR), has attracted much attention recently. Traditional Chinese Medicine (TCM) Bob ...Zhang, BVK Kumar, and David Zhang. Detecting diabetes mellitus and nonproliferative diabetic retinopathy using tongue color, texture, and geometry features. Biomedical Engineering, IEEE Transactions on, 61(2):491–501, 2014., Bob Zhang, BVK Kumar, and David Zhang. Noninvasive diabetes mellitus detection using facial block color with a sparse representation classifier. Biomedical Engineering, IEEE Transactions on, 61(4):1027–1033, 2014. etc. has proved that tongue, face and sublingual diagnosis as a noninvasive method is a reasonable way for disease detection. However, most previous works only focus on a single task (tongue, face or sublingual) for diagnosis, although different tasks may provide complementary information for the diagnosis of DM and IGR. In this paper, we propose a novel fusion method to jointly represent the tongue, face and sublingual information and discriminate between DM (or IGR) and healthy controls. Specially, the tongue, facial and sublingual images are first collected by using a non-invasive capture device. The color, texture and geometry features of these three types of images are then extracted, respectively. Finally, our so-called joint similar and specific learning (JSSL) approach is proposed to combine features of tongue, face and sublingual vein, which not only exploits the correlation but also extracts individual components among them. Experimental results on a dataset consisting of 192 Healthy, 198 DM and 114 IGR samples (all samples were obtained from Guangdong Provincial Hospital of Traditional Chinese Medicine) substantiate the effectiveness and superiority of our proposed method for the diagnosis of DM and IGR, achieving 86.07% and 76.68% in average accuracy and 0.8842 and 0.8278 in area under the ROC curves, respectively. The source code can be found in https://github.com/sasky1/JSSLreleased.
•We studied the process of extracting CLP by single factor experiment and response surface methodology.•The CLP with a concentration of 6.25–50 μg/mL significantly promoted the proliferation of ...RAW264.7 cells without showing toxic effects.•CLP significantly stimulated the phagocytosis of RAW264.7 and showed a dose-dependent effect, and significant changes in the morphology of macrophages.•CLP effectively increased the synthesis and secretion of cytokines (IL-6, TNF-α, IL-1β, and NO).
The process of extracting polysaccharides from the green algae Caulerpa lentillifera was studied by single factor experiments and response surface methodology. Additionally, the immunostimulatory activity of Caulerpa lentillifera polysaccharides (CLP) on RAW264.7 mouse macrophage was evaluated by in vitro cell experiments. The results showed that the optimal extraction conditions consisted of ultrasonification for 30 min, extraction time of 9 h, extraction temperature of 100 °C, and a ratio of water to raw material of 40:1. RAW264.7 macrophage exhibited enhanced phagocytosis with no toxic effects after treatment with CLP. In addition, CLP effectively increased the synthesis and secretion of cytokines (IL-6, TNF-α, IL-1β, and NO), whereby the secretion levels of IL-6, TNF-α, and IL-1β were 1,840.32 ± 21.03 pg/mL (50 μg/mL), 197.17 ± 3.13 ng/mL (50 μg/mL), and 1,178.35 ± 78.82 pg/mL (25 μg/mL), respectively. The polysaccharides contained in Caulerpa lentillifera have potential value for further development due to their immunological activity.
The present study isolated and characterized the barramundi (Lates calcarifer) skin collagen (BC) and tilapia (Oreochromis niloticus) skin collagen (TC). The yields of BC and TC by enzymatic ...extraction were 47.3±3.7% and 52.6±6.1% respectively, dry weight. The SDS-PAGE profile indicated both collagens were mainly type I with two different α chains. FTIR spectra and X-ray diffraction confirmed that the triple helical structure of both collagens was not affected by pepsin digestion. The denaturation (Td) and melting temperature (Tm) were 36.8 and 109.6°C for BC, 37.6 and 113.7°C for TC, measured by rheometer and DSC. This high thermal stability could be attributed to the high imino acid content (205.9 and 210.9 residues/1000 residues) of BC and TC. Fibril-forming studies indicated BC exhibited higher ability than (p<0.05) that of TC, especially under the effect of NaCl. One major characteristic of this result showed that NaCl had the markedly effects of promoting collagen forming fibrils, and electron microscopic observation corroborated this phenomenon. In general, barramundi and tilapia skin collagen with high thermal stability and good fibril-forming ability may be suitable for use as an alternative to mammalian-derived collagen in biomaterials, pharmaceuticals and cosmetics.
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