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Efficient and stable catalysts are in high demand for accelerating the oxygen evolution reaction (OER). Herein, a high-entropy sulfide (HES) of (FeCoNiCrCuAl)S@HCS with a 3D structure is successfully prepared by utilizing a simple one-step solvothermal method and employed as catalyst toward OER. The lower electronegativity of Al compared to the other metal elements and its anti-corrosion character enable an outstanding OER performance of (FeCoNiCrCuAl)S@HCS with an overpotential of 253 mV at 10 mA cm-2 and an excellent durability after 20 000 CV cycles, outperforming the commercial RuO2 and most reported metal-sulfide catalysts. Experiments coupled with theoretical calculations reveal that Al atom primarily serves as electron donor and promotes a redistribution of local electrons from Co and Cr toward adjacent Fe, Ni, and Cu sites. As a result, the Cr-Al site possesses a lowest energy barrier during the rate-determining step and works as the dominant active site for OER process. This study provides a novel insight and strategy into structural design and performance enhancement for HES materials.
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Photodetectors and imagers based on 2D layered materials are currently subject to a rapidly expanding application space, with an increasing demand for cost-effective and lightweight devices. However, the underlying carrier transport across the 2D homo- or heterojunction channel driven by the external electric field, like a gate or drain bias, is still unclear. Here, a visible-near infrared photodetector based on van der Waals stacked molybdenum telluride (MoTe2 ) and black phosphorus (BP) is reported. The type-I and type-II band alignment can be tuned by the gate and drain voltage combined showing a dynamic modulation of the conduction polarity and negative differential transconductance. The heterojunction devices show a good photoresponse to light illumination ranging from 520-2000 nm. The built-in potential at the MoTe2 /BP interface can efficiently separate photoexcited electron-hole pairs with a high responsivity of 290 mA W-1 , an external quantum efficiency of 70%, and a fast photoresponse of 78 µs under zero bias.
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Sarcoptes scabiei cause scabies in humans or sarcoptic mange in animals. Currently, information regarding vaccines against S. scabiei is limited and no commercial vaccine is available. In present study, we expressed and mixed recombinant S. scabiei serpin (rSs-serpin), recombinant S. scabiei chitinase-like protein-5 [rSs-CLP5] and -12 [rSs-CLP12] as a cocktail vaccine (three proteins mixed), and also a multi-epitope protein derived from these three S. scabiei genes was expressed as a vaccine candidate to evaluate the effects of two vaccine strategies. Four test groups (n = 12 per group) and a control group (n = 12 per group) were involved in this vaccination trial. The results showed that 91.67% (11/12) and 83.33% (10/12) of rabbits exhibited no detectable skin lesions from S. scabiei infestation in cocktail vaccine groups, whereas two multi-epitope groups produced only a few rabbits (5/12, 6/12) having no detectable skin lesions. Four test groups displayed significant increases in specific IgG antibodies (Abs) and total IgE Abs after immunized with recombinant proteins. Taken together, our data demonstrated a mixture of rSs-serpin, rSs-CLP5 and rSs-CLP12 was a promising vaccine candidate that induced robust immune protection and could significantly decrease mite populations to reduce the direct transmission between rabbits. However, vaccination with the multi-epitope protein showed limited protection in rabbits.
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Escabiosis , Serpinas , Vacunas , Animales , Humanos , Conejos , Sarcoptes scabiei , Epítopos , Escabiosis/prevención & control , Escabiosis/veterinaria , Vacunación/veterinaria , AnticuerposRESUMEN
Permanganate (Mn(VII)) is widely used as an oxidant in water treatment and usually reduced to nascent manganese dioxide (MnO2), which could promote Mn(VII) oxidation for the Mn(VII)-reactive compounds such as phenols and anilines. However, the removal of micropollutants containing diverse functional groups and the underlying mechanisms remain largely unexplored. This study reveals that Mn(VII)/nascent MnO2 was effective for the degradation of Mn(VII)-inert micropollutants, including sulfonamide antibiotics, ß-blockers and trimethoprim, with observed first-order rate constants (k'obs) of 0.126 â¼ 9 min-1 at pH 4.0. The synergetic effect of Mn(VII) and nascent MnO2 on the degradation of Mn(VII)-inert micropollutants decreased significantly when pH increased from 4.0 to 9.5. MnO2 played multiple roles in micropollutant degradation, which acted as a catalyst to promote the Mn(VII) oxidation of trimethoprim and propranolol, as well as an oxidant in propranolol degradation. Besides, Mn(III) oxidation accounted for 58% of the overall degradation of propranolol, but was not important for trimethoprim oxidation. Hydroxylated products were common products formed in Mn(VII)/MnO2. Differently, trimethoprim tended to form single-ring products via MnO2-catalyzed Mn(VII) oxidation, while propranolol preferentially formed dimers via in situ formed MnO2 oxidation. This study is the first to report that MnO2 enhances the abatement of Mn(VII)-inert micropollutants during Mn(VII)-based water treatment and unravels the multiple roles of MnO2 in micropollutant degradation by Mn(VII)/MnO2.
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Electrocatalytic water splitting has appeared to be a sustainable green technology for hydrogen and oxygen production, and noble metal-based electrocatalysts, like Pt for hydrogen evolution reaction (HER) and RuO2/IrO2 for oxygen evolution reaction (OER) have been proved to be state-of-the-art in water electrolyzers. However, high cost and scarcity of noble metals hinder large-scale applications of these electrocatalysts in practical commercial water electrolyzers. As an alternative, transition metal based electrocatalysts have attracted great attention because of the exciting catalytic performance, cost-effectiveness and abundant availability. However, their long-term stability in water splitting devices is unsatisfactory because of agglomeration and dissolution in the harsh operating environment. A possible solution to this issue is encapsulating transition metal (TM) based materials in stable and highly conductive carbon nanomaterials (CNMs) to make a hybrid of TM/CNMs, and the performance of TM/CNMs could be further enhanced by heteroatom (N-, B-, and dual N,B-) doping to carbon network in CNMs to break the carbon electroneutrality due to the different electronegativity, modulate the electronic structure to facilitate the adsorption of reaction intermediates, and promotion of efficient electron transfer to enhance the number of catalytically active sites for water splitting operation. In this review article, the recent progress of TM-based materials hybridizing with CNMs, N-CNMs, B-CNMs, and N,B-CNMs as electrocatalysts towards HER, OER as well as overall water splitting have been summarized, and the challenges and future prospects are also discussed.
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This study investigated the roles of diverse free available chlorine (FAC) species including HOCl/OCl-, H2OCl+, Cl2O, and Cl2 in the degradation of micropollutants. The degradation of 5 micropollutants was significantly affected by pH, FAC dosage, and chloride (Cl-) concentration. The reaction orders in FAC (n) of 5 micropollutants (acetaminophen, carbamazepine, naproxen, gemfibrozil, and mecoprop) ranged from 1.4 ± 0.2 to 2.1 ± 0.3 at pH 3 - 5, evidencing the importance of Cl2O and Cl2 for micropollutant abatement. A simplified method for the determination of second-order rate constants (k) of specific FAC species with micropollutants was developed. Herein, the k for neutral/dissociated forms of 5 micropollutants with Cl2 and Cl2O were determined in the ranges of 9.3 (± 0.2) × 102 â¼ 2.9 (± 0.2) × 109 M-1 s-1 and 1.8 (± 0.1) × 104 â¼ 3.7 (± 0.6) × 109 M-1 s-1, respectively. They were 4 - 7 orders of magnitude higher than those of HOCl, whereas those of OCl- and H2OCl+ were negligible. By using kinetic modeling, Cl2 was more important under acidic conditions and higher Cl- levels with contributions of 37.9 - 99.2% at pH 5 in pure water. Cl2O played a dominant role in micropollutant degradation in pure water (56.4 - 87.3%) under neutral conditions. Furthermore, both Cl2 and Cl2O played vital roles in the formation of disinfection byproducts (DBPs) during chlorination of carbamazepine and natural organic matter. This study highlights the overlooked roles of Cl2O and Cl2 in micropollutant abatement and DBP formation during chlorination.
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Contaminantes Químicos del Agua , Purificación del Agua , Halogenación , Purificación del Agua/métodos , Concentración de Iones de Hidrógeno , Cinética , Cloro , Desinfección , CarbamazepinaRESUMEN
The development of carbon materials for potassium storage is limited by their low specific capacity and poor cycling stability due to the sluggish kinetics of K ions. Herein, fucoidan-derived oxygen-rich carbon nanosheets are reported as a fantastic anode for potassium ion batteries. Attributed to its 2D porous sheet-like structure (morphology engineering), rich oxygen doping (defect engineering), and dilated graphitic layer in an amorphous structure (structure engineering), a competitive capacity of 392 mA h g-1 at 0.05 A g-1 and a long cycling span over 2500 cycles at 2 A g-1 was achieved for the carbon anode, outperforming most of the reported carbons. The kinetic analyses reveal that rich active sites and a porous nanosheet structure account for the superb rate performance and cycling stability of the material. Ex situ X-ray photoelectron spectroscopy measurements demonstrate that the introduction of C[double bond, length as m-dash]O greatly promotes K+ adsorption, and that the improvement of the C[double bond, length as m-dash]O bonds during cycling contributes to enhancement in the capacity. The fabricated potassium ion hybrid capacitor displays an exceptional energy/power density of 193 W h kg-1/22 324 W kg-1, and a promising cycling stability with 99.3% capacity retention over 2000 cycles. This work provides a large-scale synthesis strategy for preparing oxygen-rich carbon nanosheets for advanced potassium ion storage.
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Designing carbon anodes with rich heteroatoms and dilated graphitic interlayer spacing via a one-step synthesis process plays a vital role in accelerating the practical application of potassium ion batteries, but it is still a big challenge. Herein, P-doped S-rich mesoporous carbon (PSMC) is prepared by direct phosphate-assisted carbonization of carrageenan, and it exhibits excellent potassium storage capacity (449 mA h g-1 at 0.1 A g-1), superior rate performance (233 mA h g-1 at 2 A g-1) and long-term stability (97.3% capacity retention after 1000 cycles), due to the high sulfur doping (16.48 wt%) and the coexistence of ordered and disordered regions in the structure. Ex situ characterization, GITT and theoretical calculations reveal that the promotion of covalent sulfur can effectively increase the adsorption of K+ and enhance the K+ reaction kinetics. The proposed one-step synthesis strategy demonstrates the precise use of the composition in biomass, enabling large-scale production of high-performance anodes for K+ storage.
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It is a major challenge to achieve fast charging and high reversible capacity in potassium ion storing carbons. Here, we synthesized sulfur-rich graphene nanoboxes (SGNs) by one-step chemical vapor deposition to deliver exceptional rate and cyclability performance as potassium ion battery and potassium ion capacitor (PIC) anodes. The SGN electrode exhibits a record reversible capacity of 516 mAh g-1 at 0.05 A g-1, record fast charge capacity of 223 mA h g-1 at 1 A g-1, and exceptional stability with 89% capacity retention after 1000 cycles. Additionally, the SGN-based PIC displays highly favorable Ragone chart characteristics: 112 Wh kg-1at 505 W kg-1 and 28 Wh kg-1 at 14618 W kg-1 with 92% capacity retention after 6000 cycles. X-ray photoelectron spectroscopy analysis illustrates a charge storage sequence based primarily on reversible ion binding at the structural-chemical defects in the carbon and the reversible formation of K-S-C and K2S compounds. Transmission electron microscopy analysis demonstrates reversible dilation of graphene due to ion intercalation, which is a secondary source of capacity at low voltage. This intercalation mechanism is shown to be stable even at cycle 1000. Galvanostatic intermittent titration technique analysis yields diffusion coefficients from 10-10 to 10-12 cm2 s-1, an order of magnitude higher than S-free carbons. The direct electroanalytic/analytic comparison indicates that chemically bound sulfur increases the number of reversible ion bonding sites, promotes reaction-controlled over diffusion-controlled kinetics, and stabilizes the solid electrolyte interphase. It is also demonstrated that the initial Coulombic efficiency can be significantly improved by switching from a standard carbonate-based electrolyte to an ether-based one.
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BACKGROUND: Scabies is caused by burrowing of the mite Sarcoptes scabiei into the stratum corneum. Currently, diagnosis via routine skin scraping is very difficult, and information on the allergenic identification of S. scabiei remains limited. METHODS: We performed comparative analysis of the serological diagnostic potential of recombinant S. scabiei chitinase-like protein-5 (rSsCLP5) and recombinant S. scabiei chitinase-like protein-12 (rSsCLP12) by measuring the levels of serum-specific IgG and IgE antibodies (Abs) as diagnostic markers. In addition, the allergenic characteristics of rSsCLP5 and rSsCLP12 were evaluated using IgE-binding experiments and skin tests. RESULTS: The IgE Abs-based indirect enzyme-linked immunosorbent assay (ELISA) methods showed high sensitivity and specificity: the rSsCLP5-based assay had 93.5% sensitivity and 94.4% specificity; the rSsCLP12-based assay had 100% sensitivity and 98.1% specificity. The specific IgE Abs in infested mouse sera could bind rSsCLP5 and rSsCLP12. In skin tests, rabbits in the rSsCLP5 and rSsCLP12 groups and positive control (histamine) groups exhibited allergic reactions. Most test sites in the rSsCLP12 group had edema, bleeding spots, and even ulcers or scabs, but such allergy symptoms were rare in the rSsCLP5 group. Moreover, the allergic history rabbit group had more severe allergic reactions and lower levels of IgE Abs compared to the healthy rabbit group in the same protein group. CONCLUSIONS: These findings validate the use of IgE Abs to rSsCLP5 and rSsCLP12 as potentially useful markers for diagnosing scabies. Moreover, both rSsCLP5 and rSsCLP12 have allergenic properties, and the potential allergen rSsCLP12 is a stronger allergen than rSsCLP5.
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Alérgenos/inmunología , Quitinasas/genética , Quitinasas/inmunología , Inmunoglobulina E/sangre , Escabiosis/diagnóstico , Escabiosis/inmunología , Pruebas Serológicas/normas , Alérgenos/genética , Animales , Quitinasas/clasificación , Ensayo de Inmunoadsorción Enzimática/métodos , Ensayo de Inmunoadsorción Enzimática/normas , Femenino , Masculino , Ratones , Conejos , Proteínas Recombinantes/genética , Proteínas Recombinantes/inmunología , Escabiosis/genética , Sensibilidad y Especificidad , Pruebas Serológicas/métodos , Pruebas CutáneasRESUMEN
The practical application of transition metal phosphides has been hampered by the inferior rate capability and large volume change during charging and discharging processes. To address this, the construction of metal phosphide heterostructures combined with a porous carbon skeleton is a promising strategy for providing fast charge transfer kinetics. Herein, hetero-CoP/FeP nanoparticles embedded in porous carbon nanofibers (CoP/FeP@PCNFs) are obtained by coaxial electrospinning and low-temperature phosphorization processes. By employing CoP/FeP@PCNFs as the anode for sodium-ion batteries, a large reversible specific capacity (459 mA h g-1 at 0.05 A g-1), excellent rate performance (46.4% capacity retention rate at 10 A g-1 relative to 0.05 A g-1) and long-term cycling stability (208 mA h g-1 at 5 A g-1 over 1000 cycles and 73.5% capacity retention) can be obtained. By virtue of the porous structure and heterogeneous structure, the electrochemical performance of the CoP/FeP@PCNF sample was greatly improved. The porous structure can promote the ion transport and accommodate the volume expansion. Density functional theory calculation confirms that the constructed heterostructure can generate a built-in electric field and facilitate the reaction kinetics of Na+. This work provides the basic guidance for the future development of energy storage materials by designing heterostructures with a porous structure.
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Scabies is a highly contagious disease caused by Sarcoptes scabiei which burrows into stratum corneum of host's skin. In this study, after optimizing vaccination schedule, a vaccination trial is comprised of three test groups of rabbits (n = 10/group) by immunization with (1) rSsCLP5; (2) rSsCLP12; or (3) a mixture of rSsCLP5 and rSsCLP12, three biological replicates groups (n = 10/group) and three control groups (n = 10/group). Levels of specific IgG, total IgE and cytokines in sera were detected and histopathologically analyzed as indicators of vaccine effects. The results showed that 85% (17/20) of rabbits exhibited no detectable skin lesions of S. scabiei infestation in mixed protein groups compared to single protein groups with 75% (15/20) and 70% (14/20), respectively. Moreover, the deworming rates of mixed groups are increased by 10%-20% compared with that of single groups. Each of six groups immunized with rSsCLP displayed significant increases of specific IgG, total IgE, IL-10, and TNF-α. The degree of skin damage in test groups also significantly lower than that of control groups. Thus, purified rSsCLP5 and rSsCLP12 subunit cocktail vaccine induced robust immune protection and could significantly decrease mite populations to reduce the direct transmission between rabbits.
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Eimeria stiedai is an apicomplexan protozoan parasite that invades the liver and bile duct epithelial cells in rabbits and causes severe hepatic coccidiosis, resulting in significant economic losses in the domestic rabbit industry. Hepatic coccidiosis lacks the typical clinical symptoms and there is a lack of effective premortem tools to timely diagnose this disease. Therefore, in the present study we cloned and expressed the two microneme proteins i.e., microneme protein 1 (EsMIC1) and microneme protein 3 (EsMIC3) from E. stiedai and used them as recombinant antigens to develop a serodiagnostic method for an effective diagnosis of hepatic coccidiosis. The cDNAs encoding EsMIC1 and EsMIC3 were cloned and the mRNA expression levels of these two genes at different developmental stages of E. stiedai were determined by quantitative real-time PCR analysis (qRT-PCR). The immunoreactivity of recombinant EsMIC1 (rEsMIC1) and EsMIC3 (rEsMIC3) proteins were detected by Western blotting, and indirect enzyme-linked immunosorbent assays (ELISAs) based on these two recombinant antigens were established to evaluate their serodiagnostic potential. Our results showed that the proteins encoded by the ORFs of EsMIC1 (711 bp) and EsMIC3 (891 bp) were approximately 25.89 and 32.39 kDa in predicted molecular weight, respectively. Both EsMIC1 and EsMIC3 showed the highest mRNA expression levels in the merozoites stage of E. stiedai. Western blotting analysis revealed that both recombinant proteins were recognized by E. stiedai positive sera, and the indirect ELISAs using rEsMIC1 and rEsMIC3 were developed based on their good immunoreactivity, with 100% (48/48) sensitivity and 97.9% (47/48) specificity for rEsMIC1 with 100% (48/48) sensitivity and 100% (48/48) specificity for rEsMIC3, respectively. Moreover, rEsMIC1- and rEsMIC3-based indirect ELISA were able to detect corresponding antibodies in sera at days 6, 8, and 10 post E. stiedai infection, with the highest positive diagnostic rate (62.5% (30/48) for rEsMIC1 and 66.7% (32/48) for rEsMIC3) observed at day 10 post infection. Therefore, both EsMIC1 and EsMIC3 can be used as potential serodiagnostic candidate antigens for hepatic coccidiosis caused by E. stiedai.
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Antígenos de Protozoos/inmunología , Coccidiosis/diagnóstico , Eimeria/genética , Proteínas Protozoarias/genética , Pruebas Serológicas/métodos , Animales , Anticuerpos Antiprotozoarios/sangre , Anticuerpos Antiprotozoarios/inmunología , Coccidiosis/inmunología , Eimeria/inmunología , Eimeria/metabolismo , Proteínas Protozoarias/inmunología , Proteínas Protozoarias/metabolismo , ARN Mensajero/genética , ARN Mensajero/metabolismo , Conejos , Sensibilidad y Especificidad , Pruebas Serológicas/normasRESUMEN
BACKGROUND: Scabies, caused by infestation of the mite Sarcoptes scabiei, is one of the most severe ectoparasitic diseases in rabbits. Scabies seriously affects the commercial rabbit breeding, causing severe economic losses. Host resistance to S. scabiei is an important factor in further development of the rabbit industry. In the present study, we compared the host resistance to S. scabiei var. cuniculi of a new breed of domestic rabbit propagated by the Sichuan Animal Sciences Academy (QiXing rabbit, QX) compared with that of a traditional rabbit breed in the domestic rabbit industry (IRA rabbit, IRA). METHODS: Both QX and IRA rabbits were experimentally infested with live S. scabiei var. cuniculi mites for 48 h. Then, during the course of four-week experimental infestation period, the body weight of rabbits was recorded every two weeks for calculating body-weight variations in comparison to the non-infested control rabbits. Skin lesions in the foot area were assessed on weekly basis and serum samples were tested weekly for the estimation of changes in the total antibody levels (IgG, IgE and IgM). Moreover, DNA extracted from the blood samples was amplified for analysis of the genetic diversity in the major histocompatibility complex, class II, DQ Alpha (MHC-DQA) gene. RESULTS: Compared to the IRA rabbits, the QX rabbits showed a significantly higher (P < 0.05) relative body weight gain compared to the non-infested control rabbits and significantly lower (P < 0.05) scores for foot skin lesions and higher levels of IgG, IgE and IgM at weeks 1 to 4, week 2 and week 1 post-infestation, respectively. Furthermore, a polymorphism site at position 103 bp of exon two of MHC-DQA gene and a different gene frequency were found between two rabbit breeds, suggesting the genetic basis for the differential host resistance to the S. scabiei var. cuniculi between two rabbit breeds. CONCLUSIONS: The QX rabbits showed higher host resistance to S. scabiei var. cuniculi compared to the IRA rabbits at the clinical, immunological and genetic levels. These results provide a reference for the breeding of rabbits with adequately improved and sustained host resistance to scabies in the domestic rabbit industry.