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Designing efficient and stable non-noble metal electrocatalysts with good performance in reaction kinetics is desirable yet challenging for the study of methanol oxidation reaction (MOR). Herein, we have reported well-defined nanoscale nickel/nickel oxide (Ni/NiO) heterostructures supported by a three-dimensional (3D) porous graphene network (RG) via a delicate interface engineering technique. The as-prepared 3D Ni/NiO/RG composites achieve outstanding catalytic activity (79.5 mA cm

Alcohol fuels oxidation plays a significant role in carbon sustainable cycling and high-performance catalyst with a strong anti-poisoning effect is desired. Herein, Pt-Ni alloy supported on the N-doped graphene aerogel synthesized by simple freeze-drying and annealing was demonstrated to have such catalytic ability for alcohol fuel oxidation. Pt-Ni alloy particles were found uniformly dispersed over the surface of 3D N-doped graphene aerogel. High anti-poisoning ability for CO-like intermediates oxidation was demonstrated by the CO-stripping experiment. The as-prepared catalyst was found to have outstanding catalytic performance for methanol and ethanol oxidation with high catalytic activity, stability and catalytic kinetics. Compared to the control samples, the improved catalytic ability could be due to the presence of oxophilic Ni species and the support effect of 3D N-doped graphene aerogel that combined multi-advantages of large surface area, facile mass transfer, and abundant defects.

The monounsaturated fatty acid (MUFA) oleic acid (OA) has previously been shown to reverse saturated fatty acid palmitic acid (PA)-induced hepatic insulin resistance (IR). However, its underlying molecular mechanism is unclear. In addition, previous studies have also shown that the ω-3 polyunsaturated fatty acid (PUFA) eicosapentaenoic acid (EPA) reverses PA-induced muscle IR, but whether EPA plays the same role in hepatic IR and its possible mechanism involved need to be further clarified. Here, we confirmed that EPA reversed PA-induced IR in HepG2 cells and compared the proteomic changes after treatment with different free fatty acids (FFAs). A total of 234 proteins were determined to be differentially expressed after MUFA treatment. Their functions were mainly related to responses to stress and endogenous stimuli, lipid metabolic process, and protein binding. For PUFA treatment, the PA-induced expression changes of 1326 proteins could be reversed by EPA treatment, 415 of which were mitochondrial proteins, with most of the functional proteins involved in oxidative phosphorylation (OXPHOS) and tricarboxylic acid (TCA) cycle. Mechanistic studies revealed that the protein encoded by JUN and reactive oxygen species (ROS) play a role in OA- and EPA-reversed PA-induced IR, respectively. EPA or OA alleviated PA-induced abnormal adenosine triphosphate (ATP) production, ROS generation, and calcium (Ca2+) content. Importantly, H2O2-activated production of ROS increased the protein expression of JUN, further resulting in IR in HepG2 cells. Taken together, we demonstrate that ROS/JUN is a common response pathway employed by HepG2 cells toward FFA-regulated IR.

Layered two-dimensional (2D) materials have received tremendous attention due to their unique physical and chemical properties when downsized to single or few layers. Several types of layered materials, especially transition metal dichalcogenides (TMDs) have been demonstrated to be good electrode materials due to their interesting physical and chemical properties. Apart from TMDs, post-transition metal chalcogenides (PTMCs) recently have emerged as a family of important semiconducting materials for electrochemical studies. PTMCs are layered materials which are composed of post-transition metals raging from main group IIIA to group VA (Ga, In, Ge, Sn, Sb and Bi) and group VI chalcogen atoms (S, selenium (Se) and tellurium (Te)). Although a large number of literatures have reviewed the electrochemical and electrocatalytic applications of TMDs, less attention has been focused on PTMCs. In this review, we focus our attention on PTMCs with the aim to provide a summary to describe their fundamental electrochemical properties and electrocatalytic activity towards hydrogen evolution reaction (HER). The characteristic chemical compositions and crystal structures of PTMCs are firstly discussed, which are different from TMDs. Then, inherent electrochemistry of PTMCs is discussed to unveil the well-defined redox behaviors of PTMCs, which could potentially affect their efficiency when applied as electrode materials. Following, we focus our attention on electrocatalytic activity of PTMCs towards HER including novel synthetic strategies developed for the optimization of their HER activity. This review ends with the perspectives for the future research direction in the field of PTMC based electrocatalysts.

Fire zone sealing is an important approach to fire extinguishment and disaster relief. The study is aimed at investigating the distributions and evolutions of temperature and CH4 concentration fields during fire zone sealing and revealing the mechanism of sealing-induced gas explosion accidents. Firstly, the models of O2 consumption, heat production and products of coal combustion were constructed based on the Arrhenius equation of chemical reaction rate, and meanwhile the mathematical models of gases and temperature field in the sealing process were established. Besides, the variations of airflow volume, temperature and CH4 and O2 concentrations during and after fire zone sealing were numerically simulated. The results show that in the sealing process, the airflow into the fire zone gradually decreases, and air begins to flow out through the air intake at the later stage. After the completion of fire zone sealing, the temperature at fire source decreases briefly, then gradually increases and finally goes down. The temperature in the whole fire zone, except the fire source, also decreases first, then rises and finally falls gradually. The sealing raises the overall CH4 concentration in the fire zone, and the CH4 concentration at the air return side is always higher than that at the air intake side. When the sealed flow field gradually recovers to a steady flow field, the CH4 concentration goes up slowly under the influence of CH4 release. The research is of great significance for grasping the development of mine fire and the evolution of flow field in the sealing process and can provide guidance for the prevention of gas explosion accidents.

Atmospheric visibility can directly reflect the air quality. In this study, we measured water-soluble ions (WSIs), organic and element carbon (OC and EC) in PM2.5 from September 2017 to August 2018 in Urumqi, NW China. The results show that SO42−, NO3− and NH4+ were the major WSIs, together accounting for 7.32%–84.12% of PM2.5 mass. Total carbon (TC=OC+EC) accounted for 12.12% of PM2.5 mass on average. And OC/EC > 2 indicated the formation of secondary organic carbon (SOC). The levels of SO42−, NO3− and NH4+ in low visibility days were much higher than those in high visibility days. Relative humidity (RH) played a key role in affecting visibility. The extinction coefficient (bext) that estimated via Koschmieder formula with visibility was the highest in winter (1441.05 ± 739.95 Mm−1), and the lowest in summer (128.58 ± 58.00 Mm−1). The bext that estimated via IMPROVE formula with PM2.5 chemical component was mainly contributed by (NH4)2SO4 and NH4NO3. The bext values calculated by both approaches presented a good correlation with each other (R2 = 0.87). Multiple linear regression (MLR) method was further employed to reconstruct the empirical regression model of visibility as a function of PM2.5 chemical components, NO2 and RH. The results of source apportionment by Positive Matrix Factorization (PMF) model showed that residential coal combustion and vehicle emissions were the major sources of bext.

Polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) are typical persistent organic pollutants (POPs), which have high toxicity, bioaccumulation and long-distance transfer capability. Daily variation, sources of PCBs and OCPs in PM2.5 are rarely explored in polluted rural area. Here, the sources and health risks of the PCBs and OCPs were evaluated for 48 PM2.5 samples collected in winter 2017 in Wangdu, a heavy polluted rural area in the North China Plain. The average diurnal and nocturnal concentrations of Σ18PCBs and Σ15OCPs were 1.74-24.37 and 1.77-100.49, 11.67-408.81 and 16.89-865.60 pg/m3, respectively. Hexa-CBs and penta-CBs accounted for higher proportions (29.0% and 33.6%) of clean and polluted samples, respectively. Hexachlorobenzene (HCB) was the dominant contributor to OCPs with an average concentration of 116.17 pg/m3. Hexachlorocyclohexane (ΣHCHs) and dichlorodiphenyltrichloroethane (ΣDDTs) were the other two main classes in OCPs with the average concentrations of 4.33 and 15.89 pg/m3, respectively. β-HCH and p,p'-DDE were the main degradation products of HCHs and DDTs, respectively. The principal component analysis and characteristic ratio method indicated both waste incineration and industrial activities were the main sources of PCBs, contributing 76.8% and 12.7%, respectively. The loadings of OCPs were attributed to their application characteristics and the characteristic ratio method reflected a current or past use of OCPs. Health risk assessment showed that the respiratory exposure quantity of doxin-like PCBs (DL-PCBs) and the lifetime cancer risk from airborne OCPs exposure was negligible, while the other exposure modes may pose a risk to human bodies.

It is a big challenge to isolate extracellular vesicles (EVs) from human plasma because of the contamination from high abundant lipoproteins, such as high density lipoprotein (HDL) and low density lipoprotein particles (LDL). In this study, the parameters of asymmetrical flow field-flow fractionation (AF4) technology and sample preparation, including cross flow gradient, focusing time, ultrafiltration condition, sample amount and injection volume have been optimized and successfully utilized for the separation and characterization of EVs from human plasma. This study demonstrated that the great potential of AF4 in the separation of EVs from HDL and LDL in human plasma with high reproducibility and purity. This study indicated excessive focusing time in the AF4 separation and 100–300 kDa MWCO membrane based ultrafiltration in the pre-preparation will cause loss of EVs. A total of 1038 proteins have been identified in seven replicates of purified EVs from pooled human plasma sample. They are mainly enriched in extracellular exosomes, involved in extracellular matrix structural constituent, and associated with extracellular matrix-receptor interaction pathway. This study also indicated that human plasma contains more EVs than the paired serum at the same volume, and showed age- and gender-independent individual variability of the amount of EVs in human plasma. This study displayed that AF4 technique can serve as a powerful platform for the separation of EVs from human plasma, serum or human body fluids and this technology will promote the studies on EVs, such as proteomics, biomarker discovery and functions.

W2B5 powder was synthesized by the reaction between WO3 and amorphous B in NaCl/KCl flux. The results indicate that appropriate amount of NaCl/KCl flux significantly improved the completion of borothermal reduction reaction. When the weight of NaCl/KCl was 10 times that of WO3/B, pure phase W2B5 powder could be obtained at 1100 °C. The synthesized powder was composed of agglomerated nanosized particles. The oxidation resistance of the synthesized W2B5 powder was evaluated by a simultaneous thermogravimetric and differential scanning calorimetry technique.

Purpose To compare the efficacy and safety of individual devices for femoral and/or tibial graft fixation in anterior cruciate ligament (ACL) reconstruction. Methods The PubMed, Embase, Cochrane Library, and Web of Science databases were searched from inception to December 12, 2018. Randomized controlled trials comparing individual devices for ACL graft fixation were included. Bayesian network meta-analysis was performed to assess the efficacy profile using the following outcomes: Lysholm score, International Knee Documentation Committee (IKDC) category, laxity, range of motion, and Tegner score. The incidence of infection, effusion, and graft rupture for each device was reported. Results We included 57 randomized controlled trials involving 4,304 patients aged 23.8 to 40.9 years. The female proportion ranged from 0% to 100%. The length of follow-up ranged from 6 to 144 months. Of the 13 studied femoral fixation devices, none was significantly different from the others regarding the Lysholm score, IKDC category, range of motion, and Tegner score. Bioabsorbable interference screws (standardized mean difference, 1.3; 95% credible interval, 0.0-2.5) showed higher laxity than the EndoPearl at a borderline level of statistical significance, but the difference varied substantially within multiple sensitivity analyses. Infection (2.0%) was most commonly seen with the EndoPearl, whereas the bone mulch screw had the highest incidence of effusion (5.5%) and graft rupture (5.5%). For the 9 studied tibial fixation devices, no significant difference was observed in the aforementioned efficacy measurements. Bioabsorbable interference screws with staples had the highest incidence of infection (11.1%) and effusion (15.6%), whereas graft rupture was most commonly seen with the bone plug (4.0%). Conclusions Graft fixation devices in ACL reconstruction share a similar efficacy profile in terms of the Lysholm score, IKDC category, range of motion, and Tegner score but not laxity. On the other hand, safety profiles seem to vary among different devices. These findings can support surgeons, alongside their experience and preference, as well as the relative cost of each device, in delivering an individualized plan for an optimal operation. Level of Evidence Level II, meta-analysis of Level I and II studies.

Effects of the starting TiC particle size on the phase compositions, microstructures and mechanical properties of B4C–TiB2 composites prepared by reactive hot-press sintering of TiC–B mixtures were investigated. B4C–TiB2 composites were prepared from a single grade amorphous B powder (0.9 μm) and three different TiC powders (50 nm, 0.8 μm and 3.0 μm), respectively. The composites prepared from 50 nm and 3.0 μm TiC powders exhibited finer microstructures and higher hardness (29–30 GPa). The composite prepared from 0.8 μm TiC powder showed the coarsest microstructure but possessed the highest strength of 659 MPa due to its homogenous phase distribution without C impurity and abnormal grain growth that presented in the other two composites. The results indicated that the mechanical properties of B4C–TiB2 composite could be controlled by the particle size matching between TiC and B powders.

Xinfeng capsule is a traditional Chinese medicine compound, which has been clinically used for more than 20 years in the treatment of rheumatoid arthritis (RA), ankylosing spondylitis, osteoarthritis and its extracurricular lesions. However, the molecular role of XFC in the treatment of RA remains unclear.This study aims to explore the efficacy and potential mechanism of XFC through retrospective data mining analysis, animal experiments and cell experiments.The effect of XFC on clinical laboratory indexes of RA patients was observed using data mining techniques combined with association rule analysis and a random walk model. Afterwards, a rat model of adjuvant arthritis (AA) was established with Freund's complete adjuvant, followed by the observation of pathological changes in synovial tissues and the ultrastructure of synoviocytes. A RA cell model was constructed by inducing fibroblast-like synoviocytes (FLSs) with tumor necrosis factor-alpha (TNF-α) to assess the effects of XFC-containing serum on inflammation and oxidative stress through long non-coding RNA LINC00638.In retrospective data mining, XFC effectively reduced immune inflammation and increase the level of antioxidant enzymes in RA patients. Subsequently, animal experiments showed that XFC significantly repressed immune inflammation, oxidative stress, synovial hyperplasia, and cartilage destruction, while improving the ultrastructure of synoviocytes in AA rats. XFC-containing serum diminished the proliferation of TNF-α-induced RA-FLSs, increased LINC00638 expression (P＜0.01), decreased interleukin-6 (IL-6), IL-17, reactive oxygen species (ROS) and reactive nitrogen species (RNS) levels (P＜0.01), and increased the protein expression of nuclear factor erythrocyte 2-related factor 2 (Nrf2), heme oxygenase 1 (HO-1), and superoxide dismutase 2 (SOD2) (P＜0.01). Furthermore, rescue experiments manifested that XFC-containing serum reversed the effects of silencing LINC00638 on inflammation and oxidative stress in RA-FLSs.XFC inhibits inflammation and oxidative stress in RA by up-regulating LINC00638 and activating Nrf2/HO-1 pathway.

High health risks of vanadium (V) released by the mining of vanadium titanomagnetite (VTM) have been widely recognized, but little is known about the risks and microbial community responses of V pollution as a consequence of the stone coal mining (SCM), another important resource for V mining. In this study, the topsoils and the profile soils were collected from the agricultural soils around a typical SCM in Hunan Province, China, with the investigation of ecological, health risks and microbial community structures. The results showed that ∼97.6% of sampling sites had levels of total V exceeding the Chinese National standard (i.e., 130 mg/kg), and up to 41.1% of V speciation in the topsoils was pentavalent vanadium (V(V)). Meanwhile, the proportions of HQ 1 and 0.6-1 in the topsoils were ∼8.3% and ∼31.0% respectively, indicating that V might pose a non-carcinogenic risk to children. In addition, the microbial community varied between the topsoils and the profile soils. Both sulfur-oxidizing bacteria (e.g. Thiobacillus, MND1, Ignavibacterium) and sulfate-reducing bacteria (e.g. Desulfatiglans, GOUTB8, GOUTA6) might have been involved in V(V) reductive detoxification. This study helps better understand the pollution and associated risks of V in the soils of SCM and provides a potential strategy for bioremediation of the V-contaminated environment.

Source apportionment is critical but remains largely unknown for heavy metals in the soil surrounding black shale mining areas. Herein, the distribution, potential hazards, and sources of heavy metals in the soil around a black shale post-mining site were investigated. The content of Cadmium (Cd) in topsoil samples (0.77-50.29 mg/kg, N = 84) all exceeded the Chinese agricultural soil standard (0.3 mg/kg). The majority of Cd in the soil existed in the mobile fraction posing a high potential risk to the local ecosystem. and Zn and V in soils existed in the residual form. The percentages of HQ

To understand zooplankton community changes in the context of climate change and anthropogenic disturbances, we analyzed mesozooplankton samples from four seasons in the subtropical Daya Bay, which is susceptible to perceived disturbances in the South China Sea. The zooplankton community was found to be divided into two clusters, namely the Outer-bay Cluster (OC) comprising Noctiluca scintillans, Temora turbinata, and Paracalanus spp., and the Inner-bay Cluster (IC) which was dominated by Pseudevadne tergestina, Oikopleura rufescens, and Paracalanus spp. The OC was recorded in waters with low Chl a concentrations and high salinity, coinciding with open seawater intrusion. The IC occurred in waters with high Chl a concentrations, low salinity, with terrestrial inputs from the Dan'ao River. The dominant cladoceran species has changed in spring from Penilia avirostris to Pseudevadne tergestina owing to suitable temperature conditions and the low wind speed in this region. Most of the keystone species recorded during all seasons were found to be copepods based on co-occurrence network analysis. Numbers of keystone jellyfish (cnidaria) species, such as Geryonia proboscidalis, Chelophyes contorta, and Aeginura grimaldi were significantly higher in summer than in other seasons due to a low-temperature seawater intrusion, which can result in the highest stability of community structures and affect coastal food webs and fishery resources. Our results highlight that zooplankton community succession may occur with long-term temperature changes in the subtropical Daya Bay under global climate change conditions.

Supercapacitors, which can supply superior energy density compared to conventional dielectric capacitors and higher power density than batteries, have attracted considerable attention as a promising energy storage device. However, cycle performance and specific energy density are still key factors limiting its practical applications. This work reports a facile synthesis of high-performance asymmetric supercapacitors with hybrid nickel phosphides/nickel foam as positive electrode and biomass-based sulfur-doped hierarchical porous activated carbon as negative electrodes. It demonstrates a novel one-step colloid synthesis of nickel phosphides directly on commercial nickel foam as only nickel source. The obtained electrode exhibits satisfactory specific capacity of 1032 C g−1 (2293 F g−1) at 1 A g−1 and cyclic stability over 10,000 cycles. Most importantly, the fabricated asymmetric supercapacitor devices show excellent cyclic stability with 85.7% capacitance retention after 10,000 cycles and deliver a maximum energy density of 42.2 Wh kg−1 at 741.1 W kg−1 power density. To the best of our knowledge, the assembled device in this report has absolute advantages in fields requiring simultaneous high energy density and long-term operation at high current density. These promising results demonstrate the possibility of a facile synthesis of efficient asymmetric supercapacitors with high electrochemical response and cycling stability.

Proton-binding study of humic acid (HA) is critical for describing and modeling the binding mechanism of HA with heavy metals. However, little is known about the intrinsic relationship between protonation behavior and HA characteristics, especially in sediments. In this study, HA was extracted from sediments and combination of spectrographic titration with parallel factor analysis, Gaussian fitting model and two-dimensional correlation spectroscopy analysis was developed as a novel in-situ tool. Results indicated that the intensity changes of fluorophores of sediment HA might be dependent on the structure characteristics (fused or non-fused ring) of phenolic species in the protonation process. Compared with phenolic groups (A1, 5.27 ± 0.05 eV; A3, 3.91 ± 0.02 eV), the carboxyl groups (A2, 4.65 ± 0.03 eV) exhibited greater contribution in the response of chromophores to the protonation process of sediment HA. Furthermore, proton binding to sediment HA first occurred in carboxyl groups and then in phenolic groups. The combined technique is a promising approach for the examination of the binding sites, binding capacities, and binding order in proton-HA binding process under environmental concentrations. Importantly, this method is a sensitive, effective and non-destructive technique without any need pre-concentrate.

As a major source of fine particles, open biomass burning can affect climate and the hydrological cycle via the formation of cloud condensation nuclei (CCN) and their deposition. This study investigated the effect of aerosol size and chemical composition (water-soluble compounds, elemental carbon, and organic carbon) on CCN activation during the complete combustion of six commonly used crop (rice, wheat, corn, soybean, and cotton) and leaf residues in a simulation chamber developed for this study. Geometric mean diameters (GMD) of emitted primary particles ranged from 68 to 130 nm and water-soluble compound (WSC) content ranged from 33 to 50%. Although GMDs and WSCs possessed similar temporal tendencies during the combustion process, their average values were dependent on the type of biomass. Number concentration ratios of CCN and particle (CCN/CN) ranged from 1.4–2.1% and 5.8–8.3% at supersaturations of 0.2% and 1.0%, respectively. The CCN/CN value increased during the combustion process when the GMD and WSC content increased. Correlation coefficients for GMD and CCN activation ranged from 0.62 to 0.93, while correlations for WSC and CCN activation ranged from 0.33 to 0.95. Soybean biomass had the highest correlations for both GMD and WSC with CCN activation at various supersaturations. These results suggest that the size and chemical composition of biomass aerosols are important in CCN formation, while the aerosol size has a higher impact.

The electrochemical properties of layered Li-rich oxide Li1.2Ni0.13Co0.13Mn0.54O2 (LLO) can be enhanced by a facile NaF surface modification. We have clarified by XPS, HR-TEM and HAADF-STEM analyses that the mechanism is the formations of a gradient coating layer Na1-xLixF and a gradient LLO surface Li1.2-xNaxNi0.13Co0.13Mn0.54O2 via a Li+/Na+ exchange reaction. The exchange reaction occurs at the Li-slabs of LLO down to a depth of less than 15 nm. After such a double gradient surface modification, the LLO displays markedly improved cycle life and rate capability as well as suppressed voltage decay. It exhibits a capacity retention of 85% beyond 1000 cycles at 10 C and a voltage decay of only 0.0021 V per cycle at 0.5 C, revealing great application prospects in energy storage materials.

Liquid N2 could be injected into goaf to decrease temperature and prevent spontaneous combustion during mining. A working face at Liangbaosi coal mine was adopted for study. Firstly, a mathematical model for calculating the temperature field in goaf was developed and field tests without injection of liquid N2 were conducted to validate the model. Comparable development trends and hot zones between the simulation and field measurements were found. The hot zones were located about 35–45 m behind the workface on the air-return and air-intake sides in the goaf. Then the model was employed to simulate the time development of temperature distribution in the goaf with injection of liquid N2 from different locations. It was observed that a low-temperature cooling zone (