A two-dimensional iron-doped carbon-based nanoenzyme with catalase-like activity for the detection of alkaline phosphatase and ascorbate oxidase.

Herein, we successfully synthesized two-dimensional iron-doped carbon-based nanosheets (Fe-N800 CS) with catalase-like activity through doping Fe into Zn MOF and introducing graphitic C3N4 (g-C3N4). The interaction of the Fe-N800 CS with hydrogen peroxide could generated abundant reactive oxygen species (ROS) and further oxidize o-Phenylenediamine (OPD) to 2,3-diaminophenazine (DAP) which has constant fluorescence at 560 nm. Ascorbic acid (AA) could be generated via the hydrolysis reaction between alkaline phosphatase (ALP) and ascorbic acid 2-phosphate (AAP). AA can be oxidized to dehy-droascorbic acid (DHA) by ROS, and then combined with OPD to generate 3-(1,2-dihydroxyethyl)furo[3,4b]-quinoxaline (QXD) with fluorescence at 440 nm, which could increase as the concentration of AA enhanced. DHA could also be generated through oxidation of AA by ascorbate oxidase (AAO). Thus, by monitoring the fluorescence ratio (I560/I440), a ratiometric fluorescence biosensing platform for ALP and AAO was established with the linear ranges in 0.2-10 U/L and 1-60 U/L, respectively. The limit of detection for ALP and AAO were 0.12 U/L and 0.59 U/L. Furthermore, the biosensing platform was successfully applied for the detection of ALP and AAO activity in human serum samples. This work provides a potential tool for future biomedical diagnostics.

A novel self-assembled dual-emissive ratiometric fluorescent nanoprobe for alkaline phosphatase sensing.

BACKGROUND: Alkaline phosphatase (ALP) is widely found in various organs and tissues of the human body which could assist in the verification of the presence of various diseases through its content in the blood. In the past few years, many analytical methods for ALP activity assays have been explored. However, a simple and economical method with high sensitivity and specificity also remains great challenge. Therefore, the development of sensitive and efficient approach for ALP analysis is of great significance in biomedical studies. RESULTS: Herein, we constructed a highly sensitive and label-free ratiometric fluorometric biosensing platform for the determination of ALP activity, which utilizing lysozyme(Ly)-functionalized 5-methyl-2-thiouracil(MTU)-modified gold nanoclusters (MTU-Ly@Au NC) and poly-dopamine (PDA) as signal indicators. Dopamine (DA) can self-polymerizes to form PDA under alkaline conditions that can further quenched the fluorescence of MTU-Ly@Au NC at 525 nm due to fluorescence resonance energy transfer (FRET) and absorption competition quenching (ACQ) effects. In this process, the PDA fluorescence intensity at 325 nm was nearly unchanged. After the addition of ALP, ascorbic acid (AA) which can alleviate the self-polymerization process of DA was generated from the substrate ascorbic acid 2-phosphate (AAP), thus changing ratiometric fluorescence intensity of I525/I325. Hence, by monitoring the fluorescence ratio (I525/I325), a ratiometric fluorescence biosensing platform for ALP was established with the linear calibration in the range of 0.5-8 U L-1 and the limit of detection of 0.157 U L-1. SIGNIFICANCE: This work not only synthesized a novel fluorescence probe with simple preparation and low cost for ALP which has excellent anti-interference properties and selectivity. Furthermore, this biosensing platform was successfully applied for the determination of ALP activity in human serum samples. This work provided a potential tool for biomedical diagnostics in the future.

MIL-100(Fe) Supported Pt-Co Nanoparticles as Active and Selective Heterogeneous Catalysts for Hydrogenation of 1,3-Butadiene.

Superior catalytic performance for selective 1,3-butadiene (1,3-BD) hydrogenation can usually be achieved with supported bimetallic catalysts. In this work, Pt-Co nanoparticles and Pt nanoparticles supported on metal-organic framework MIL-100(Fe) catalysts (MIL=Materials of Institut Lavoisier, PtCo/MIL-100(Fe) and Pt/MIL-100(Fe)) were synthesized via a simple impregnation reduction method, and their catalytic performance was investigated for the hydrogenation of 1,3-BD. Pt1Co1/MIL-100(Fe) presented better catalytic performance than Pt/MIL-100(Fe), with significantly enhanced total butene selectivity. Moreover, the secondary hydrogenation of butenes was effectively inhibited after doping with Co. The Pt1Co1/MIL-100(Fe) catalyst displayed good stability in the 1,3-BD hydrogenation reaction. No significant catalyst deactivation was observed during 9 h of hydrogenation, but its catalytic activity gradually reduces for the next 17 h. Carbon deposition on Pt1Co1/MIL-100(Fe) is the reason for its deactivation in 1,3-BD hydrogenation reaction. The spent Pt1Co1/MIL-100(Fe) catalyst could be regenerated at 200 °C, and regenerated catalysts displayed the similar 1,3-BD conversion and butene selectivity with fresh catalysts. Moreover, the rate-determining step of this reaction was hydrogen dissociation. The outstanding activity and total butene selectivity of the Pt1Co1/MIL-100(Fe) catalyst illustrate that Pt-Co bimetallic catalysts are an ideal alternative for replacing mono-noble-metal-based catalysts in selective 1,3-BD hydrogenation reactions.

Blood lead levels of children in urban and suburban areas in China (1997-2015): Temporal and spatial variations and influencing factors.

Blood lead (Pb) poisoning is a worldwide heath problem, especially in developing countries. As the largest developing country in the world, China faces severe health challenges, in particular the threat of blood Pb poisoning. In this study, the temporal trend of Chinese children's blood lead levels (BLLs) and blood lead poisoning incidence (BLPI) (percentage of BLL>100µg/L) and its influencing factors were investigated. We collected articles on children's BLLs published from 1997 to 2017 with sampling time from 1997 to 2015 by searching the databases of VIP Medical Information System (VMIS), China National Knowledge Infrastructure (CNKI) and Wanfang Data. After a rigorous investigation, 259 articles with eligible inclusion criteria were reviewed. Meanwhile, the data of Pb concentrations in the soil of 23 cities and the annual mean PM10 (particulate matter<10µm) concentrations of 24 provincial cities were collected. The temporal trend of children's BLLs and BLPIs could be divided into three stages: upward trend from 1997 to 2000, downward trend from 2001 to 2013, and upward trend from 2014 to 2015. The decline of BLLs from 2001 was primarily due to the phasing out of leaded gasoline since 2000 in China, while the descending air quality could explain the upward trend of BLLs in the period from 2014 to 2015. The correlation and regression analysis indicated that soil and air were two major pathways of Pb exposure for children in China. Although a noticeable decrease has been shown, the Chinese children's BLLs were still significantly higher than the levels of developed countries. We highly recommended that the critical value of blood Pb poisoning should be lowered to 50µg/L in China. Guidelines on the prevention and management of blood Pb poisoning are needed in China.

Lead in Chinese villager house dust: Geographical variation and influencing factors.

House dust has been recognized as an important contributor to Pb exposure of children. Here we conducted a comprehensive study to investigate geographical variation of Pb in Chinese villager house dust. The influences of outdoor soil Pb concentrations, dates of construction, house decoration materials, heating types, and site specific pollution on Pb concentrations in house dust were evaluated. The concentrations of Pb in 477 house dust samples collected from twenty eight areas throughout China varied from 12 to 2510 mg/kg, with a median concentration of 42 mg/kg. The median Pb concentrations in different geographical areas ranged from 16 (Zhangjiakou, Hebei) to 195 mg/kg (Loudi, Hunan). No correlations were found between the house dust Pb concentrations and the age of houses, as well as house decoration materials. Whereas outdoor soil, coal combustion, and site specific pollution may be potential Pb sources. Principal component analysis (PCA) confirmed that elemental compositions of the house dust were controlled by both anthropogenic and geogenic sources. Using scanning electron microscopy (SEM), the Pb bearing particles in the house dust were also studied.

In vitro bioaccessibility of lead in surface dust and implications for human exposure: A comparative study between industrial area and urban district.

In this study, ground surface dust samples from two contrasting areas, a former zinc smelting area in Guizhou Province and a common urban district in Wuhan city, Hubei Province, China, were assessed for in vitro Pb bioaccessibility using a physiologically based extraction test (PBET). Extremely elevated concentrations of Pb (220-6348 mg/kg) and other trace metals were observed in the zinc smelting area. While moderate high metal concentrations (79-1544 mg/kg of Pb) in the urban dusts were attributed to various urban activities, coal combustion and traffic emissions. Lead bioaccessibility in the stomach-phase varied from 17.6 to 76.1% and no significant difference was found between industrial and urban dust samples. Compared with the stomach-phase, Pb bioaccessibility in the more alkaline intestinal-phase was considerably lower (1.2-21.8%). A significantly negative correlation was found between dust Ca concentrations and Pb bioaccessibility in the intestinal-phase, suggesting that Ca plays an important role in reducing the bioaccessible Pb in the intestinal-phase. The estimated Pb exposure based on gastric bioaccessible Pb was 13.9 and 1.8 µg/kg day for children living in the industrial and urban areas, respectively, accounting for 85% and 41% of their corresponding total Pb exposure.

Response of magnetic properties to heavy metal pollution in dust from three industrial cities in China.

Magnetic method is a reliable and powerful technique for identification of the relative contribution of industrial pollutants. However, it has not been fully applied in urban area impacted by non-ferrous metal (NFM) smelting/processing activities. The aim of this study is to explore the applicability of magnetic methods for detecting heavy metal contamination in dust from three NFM smelting/processing industrial cities (Ezhou, Zhuzhou, and Hezhang) in China. The enhancements of magnetic susceptibility (MS) and saturation isothermal remanent magnetization (SIRM) together with heavy metals were significant in the studied areas in comparison with the background values. Scanning electron microscope (SEM) analysis revealed that magnetic particles in dust from Ezhou were dominated by spherules, while those from Zhuzhou and Hezhang were mainly consisted of irregular-shaped particles. κ-T curves and X-ray diffraction (XRD) analyses indicated that the magnetic particles from Ezhou were dominated by magnetite and metallic iron, whereas those from Zhuzhou and Hezhang were consisted of magnetite and hematite. Our study indicates that magnetic properties of the dust are sensitive to the NFM smelting/processing related heavy metal pollutants. However, the relationship between magnetic parameters and heavy metals was influenced by the presence of metallic iron particles and multi-sources of metal pollutants.

The relationship between magnetic parameters and heavy metal contents of indoor dust in e-waste recycling impacted area, Southeast China.

Environmental contamination due to uncontrolled e-waste recycling is an emerging global problem. The aim of this study is to test the applicability of magnetic methods for detecting the metal pollutants emitted from e-waste recycling activities. Dust samples collected from a typical e-waste recycling region in Guiyu, Guangdong Province, China, were investigated using magnetic, geochemical, micro-morphological and mineralogical analysis. The values of mass-specific susceptibility (χ) and saturation isothermal remanent magnetization (SIRM) in dusts from e-waste recycling impacted areas ranged from 101 to 636×10(-8) m(3) kg(-1) and from 10.5 to 85.2×10(-3) Am(2) kg(-1), respectively. There was a significant correlation between SIRM and χ (r(2)=0.747, p<0.001), indicating that ferrimagnetic minerals were dominating χ in the dust samples. The values of χ(fd)% varied from 2.6 to 4.6% with a mean of 3.4%, which suggested that magnetic carriers in the dusts are predominately coarse-grained particles. Two shapes of magnetic particles, spherule (10-150 µm) and angular-shaped particles (30-300 µm), were identified by scanning electron microscope (SEM) and energy dispersive X-ray spectrometer (EDX) analyses. κ-T curves, magnetic hysteresis loops and X-ray diffraction (XRD) analysis indicated that these magnetic particles were magnetite and goethite. There were significant correlations between SIRM and heavy metals (especially Cd, Co, Fe, Ni and Zn) as well as the Tomlinson pollution load index (PLI) of the dust, indicating that SIRM can be used as an efficient proxy for metal pollution in the e-waste recycling impacted area.

High levels of antimony in dust from e-waste recycling in southeastern China.

Environmental contamination due to uncontrolled e-waste recycling is an emerging global issue. Antimony (Sb) is a toxic element used in semiconductor components and flame retardants for circuit board within electronic equipment. When e-waste is recycled, Sb is released and contaminates the surrounding environment; however, few studies have characterized the extent of this problem. In this study, we investigated Sb and arsenic (As) distributions in indoor dust from 13 e-waste recycling villages in Guiyu, Guangdong Province, southeastern China. Results revealed significantly elevated concentrations of Sb (6.1-232 mg/kg) in dust within all villages, which were 3.9-147 times higher than those from the non e-waste sites, indicating e-waste recycling was an important source of Sb pollution. On the contrary, As concentrations (5.4-17.7 mg/kg) in e-waste dusts were similar to reference values from the control sites. Therefore, dusts emitted from e-waste recycling may be characterized by high Sb/As ratios, which may help identify the contamination due to the e-waste recycling activities.