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1.
J Am Chem Soc ; 146(4): 2426-2434, 2024 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-38228289

RESUMEN

The molecular details of an electrocatalytic interface play an essential role in the production of sustainable fuels and value-added chemicals. Many electrochemical reactions exhibit strong cation-dependent activities, but how cations affect reaction kinetics is still elusive. We report the effect of cations (K+, Li+, and Ba2+) on the interfacial water structure using second-harmonic generation (SHG) and classical molecular dynamics (MD) simulation. The second- (χH2O(2)) and third-order (χH2O(3)) optical susceptibilities of water on Pt are smaller in the presence of Ba2+ compared to those of K+, suggesting that cations can affect the interfacial water orientation. MD simulation reproduces experimental SHG observations and further shows that the competition between cation hydration and interfacial water alignment governs the net water orientation. The impact of cations on interfacial water supports a cation hydration-mediated mechanism for hydrogen electrocatalysis; i.e., the reaction occurs via water dissociation followed by cation-assisted hydroxide/water exchange on Pt. Our study highlights the role of interfacial water in electrocatalysis and how innocent additives (such as cations) can affect the local electrochemical environment.

2.
Nat Mater ; 22(4): 503-510, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36781952

RESUMEN

When an electrode contacts an electrolyte, an interfacial electric field forms. This interfacial field can polarize the electrode's surface and nearby molecules, but its effect can be countered by an applied potential. Quantifying the value of this countering potential ('potential of zero charge' (pzc)) is, however, not straightforward. Here we present an optical method for determining the pzc at an electrochemical interface. Our approach uses phase-sensitive second-harmonic generation to determine the electrochemical potential where the interfacial electric field vanishes at an electrode-electrolyte interface with Pt-water as a model experiment. Our method reveals that the pzc of the Pt-water interface is 0.23 ± 0.08 V versus standard hydrogen electrode (SHE) and is pH independent from pH 1 to pH 13. First-principles calculations with a hybrid explicit-implicit solvent model predict the pzc of the Pt(111)-water interface to be 0.23 V versus SHE and reveal how the interfacial water structure rearranges as the electrode potential is moved above and below the pzc. We further show that pzc is sensitive to surface modification; deposition of Ni on Pt shifts the interfacial pzc in the cathodic direction by ~360 mV. Our work demonstrates a materials-agnostic approach for quantifying the interfacial electrical field and water orientation at an electrochemical interface without requiring probe molecules and confirms the long-held view that the interfacial electric field is more intense during hydrogen electrocatalysis in alkaline than in acid.

3.
Chem Rev ; 122(6): 6117-6321, 2022 03 23.
Artículo en Inglés | MEDLINE | ID: mdl-35133808

RESUMEN

Hydrogen energy-based electrochemical energy conversion technologies offer the promise of enabling a transition of the global energy landscape from fossil fuels to renewable energy. Here, we present a comprehensive review of the fundamentals of electrocatalysis in alkaline media and applications in alkaline-based energy technologies, particularly alkaline fuel cells and water electrolyzers. Anion exchange (alkaline) membrane fuel cells (AEMFCs) enable the use of nonprecious electrocatalysts for the sluggish oxygen reduction reaction (ORR), relative to proton exchange membrane fuel cells (PEMFCs), which require Pt-based electrocatalysts. However, the hydrogen oxidation reaction (HOR) kinetics is significantly slower in alkaline media than in acidic media. Understanding these phenomena requires applying theoretical and experimental methods to unravel molecular-level thermodynamics and kinetics of hydrogen and oxygen electrocatalysis and, particularly, the proton-coupled electron transfer (PCET) process that takes place in a proton-deficient alkaline media. Extensive electrochemical and spectroscopic studies, on single-crystal Pt and metal oxides, have contributed to the development of activity descriptors, as well as the identification of the nature of active sites, and the rate-determining steps of the HOR and ORR. Among these, the structure and reactivity of interfacial water serve as key potential and pH-dependent kinetic factors that are helping elucidate the origins of the HOR and ORR activity differences in acids and bases. Additionally, deliberately modulating and controlling catalyst-support interactions have provided valuable insights for enhancing catalyst accessibility and durability during operation. The design and synthesis of highly conductive and durable alkaline membranes/ionomers have enabled AEMFCs to reach initial performance metrics equal to or higher than those of PEMFCs. We emphasize the importance of using membrane electrode assemblies (MEAs) to integrate the often separately pursued/optimized electrocatalyst/support and membranes/ionomer components. Operando/in situ methods, at multiscales, and ab initio simulations provide a mechanistic understanding of electron, ion, and mass transport at catalyst/ionomer/membrane interfaces and the necessary guidance to achieve fuel cell operation in air over thousands of hours. We hope that this Review will serve as a roadmap for advancing the scientific understanding of the fundamental factors governing electrochemical energy conversion in alkaline media with the ultimate goal of achieving ultralow Pt or precious-metal-free high-performance and durable alkaline fuel cells and related technologies.


Asunto(s)
Suministros de Energía Eléctrica , Protones , Hidrógeno/química , Oxígeno/química , Agua
4.
Inorg Chem ; 61(37): 14824-14832, 2022 Sep 19.
Artículo en Inglés | MEDLINE | ID: mdl-36074721

RESUMEN

Basal plane-functionalized NbS2 nanosheets were obtained using in situ photolysis to generate the coordinatively unsaturated organometallic fragment cyclopentadienyl manganese(I) dicarbonyl (CpMn(CO)2). Under UV irradiation, a labile carbonyl ligand dissociates from the tricarbonyl complex, creating an open coordination site for bonding between the Mn atom and the electron-rich sulfur atoms on the surface of the NbS2 nanosheets. In contrast, no reaction is observed with 2H-MoS2 nanosheets under the same reaction conditions. This difference in reactivity is consistent with the electronic structure calculations, which indicate stronger bonding of the organometallic fragment to electron-poor, metallic NbS2 than to semiconducting, electron-rich MoS2. X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared (FTIR) spectroscopy, and powder X-ray diffraction (PXRD) were used to characterize the bonding between Mn and S atoms on the surface-functionalized nanosheets.

5.
Proc Natl Acad Sci U S A ; 115(27): 6946-6951, 2018 07 03.
Artículo en Inglés | MEDLINE | ID: mdl-29915092

RESUMEN

Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO2 grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm-2 was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of a buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor-electrocatalyst junction behaviors in the presence of a poor semiconducting material.

6.
J Proteome Res ; 18(3): 1218-1227, 2019 03 01.
Artículo en Inglés | MEDLINE | ID: mdl-30592618

RESUMEN

Alzheimer's disease (AD) is regarded as a metabolic disorder, and more attention has been paid to brain metabolism. However, AD may also affect metabolism in the peripheral organs beyond the brain. In this study, therefore, we investigated metabolic changes in the liver, kidney, and heart of amyloid precursor protein/presenilin 1 (APP/PS1) mice at 1, 5, and 10 months of age by using 1H NMR-based metabolomics and chemometrics. Metabolomic results reveal that the liver was the earliest affected organ in APP/PS1 mice during amyloid pathology progression, followed by the kidney and heart. Moreover, a hypometabolic state was found in the liver of APP/PS1 mice at 5 months of age, and the disturbed metabolites were mainly involved in energy metabolism, amino acid metabolism, nucleic acid metabolism, as well as ketone and fatty acid metabolism. In conclusion, our results suggest that AD is a systemic metabolic dysfunction, and hepatic metabolic abnormality may reflect amyloid pathology progression.


Asunto(s)
Enfermedad de Alzheimer/genética , Encefalopatías Metabólicas/genética , Hígado/metabolismo , Presenilina-1/metabolismo , Enfermedad de Alzheimer/complicaciones , Enfermedad de Alzheimer/metabolismo , Enfermedad de Alzheimer/patología , Precursor de Proteína beta-Amiloide/genética , Precursor de Proteína beta-Amiloide/metabolismo , Animales , Encefalopatías Metabólicas/complicaciones , Encefalopatías Metabólicas/metabolismo , Encefalopatías Metabólicas/patología , Modelos Animales de Enfermedad , Humanos , Riñón/metabolismo , Hígado/patología , Metabolómica/métodos , Ratones , Miocardio/metabolismo , Especificidad de Órganos/genética , Presenilina-1/genética
7.
J Proteome Res ; 18(11): 3944-3954, 2019 11 01.
Artículo en Inglés | MEDLINE | ID: mdl-31553190

RESUMEN

Antibiotic-induced microbial perturbations alter host metabolism and affect host physiology. In this study, we aimed to investigate the effects of vancomycin (Vanc) and ciprofloxacin/metronidazole (CiMe) exposures on the gut microbiome and metabolome in the colonic content and tissue samples from advanced-stage type 1 diabetic (AST1D) rats and age-matched controls (AMCs) using 16S ribosomal RNA gene sequencing and nuclear magnetic resonance-based metabolomics. The results show that antibiotic effects on the gut microbiota were stronger in AMC rats relative to AST1D rats. These microbial alterations were accompanied by a series of metabolic changes, including energy metabolism, short-chain fatty acid metabolism, and amino acid metabolism. We found that AMC rats had a more notable metabolic response to antibiotic exposure than AST1D rats. Additionally, Vanc had a stronger impact on the gut microbiota and host metabolic phenotype versus CiMe. Therefore, our results reveal that antibiotic-induced shifts in the gut microbiome and metabolome are different between AST1D and AMC rats. If confirmed in human studies, these findings suggest that diabetic patients may need a specific strategy for antibiotic use in clinical practice.


Asunto(s)
Antibacterianos/farmacología , Diabetes Mellitus Tipo 1/metabolismo , Microbioma Gastrointestinal/efectos de los fármacos , Metaboloma/efectos de los fármacos , Metabolómica/métodos , Animales , Bacterias/clasificación , Bacterias/genética , Colon/efectos de los fármacos , Colon/metabolismo , Metabolismo Energético/efectos de los fármacos , Heces/microbiología , Microbioma Gastrointestinal/genética , Humanos , Masculino , Fenotipo , ARN Ribosómico 16S/genética , Ratas Sprague-Dawley
8.
Nano Lett ; 18(1): 546-552, 2018 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-29236505

RESUMEN

A magnetic, metallic inverse opal fabricated by infiltration into a silica nanosphere template assembled from spheres with diameters less than 100 nm is an archetypal example of a "metalattice". In traditional quantum confined structures such as dots, wires, and thin films, the physical dynamics in the free dimensions is typically largely decoupled from the behavior in the confining directions. In a metalattice, the confined and extended degrees of freedom cannot be separated. Modeling predicts that magnetic metalattices should exhibit multiple topologically distinct magnetic phases separated by sharp transitions in their hysteresis curves as their spatial dimensions become comparable to and smaller than the magnetic exchange length, potentially enabling an interesting class of "spin-engineered" magnetic materials. The challenge to synthesizing magnetic inverse opal metalattices from templates assembled from sub-100 nm spheres is in infiltrating the nanoscale, tortuous voids between the nanospheres void-free with a suitable magnetic material. Chemical fluid deposition from supercritical carbon dioxide could be a viable approach to void-free infiltration of magnetic metals in view of the ability of supercritical fluids to penetrate small void spaces. However, we find that conventional chemical fluid deposition of the magnetic late transition metal nickel into sub-100 nm silica sphere templates in conventional macroscale reactors produces a film on top of the template that appears to largely block infiltration. Other deposition approaches also face difficulties in void-free infiltration into such small nanoscale templates or require conducting substrates that may interfere with properties measurements. Here we report that introduction of "spatial confinement" into the chemical fluid reactor allows for fabrication of nearly void-free nickel metalattices by infiltration into templates with sphere sizes from 14 to 100 nm. Magnetic measurements suggest that these nickel metalattices behave as interconnected systems rather than as isolated superparamagnetic systems coupled solely by dipolar interactions.

9.
J Am Chem Soc ; 140(37): 11647-11654, 2018 09 19.
Artículo en Inglés | MEDLINE | ID: mdl-30145888

RESUMEN

In water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs), charge recombination competes with catalytic water oxidation to determine the overall efficiency of the system. The kinetics of these processes have been difficult to understand because transient absorbance (TA) experiments typically show nearly complete charge recombination on the submillisecond time scale; in contrast, electrochemical measurements such as open circuit photovoltage decay suggest a charge recombination time scale that is 2-3 orders of magnitude longer. Here we explore these processes with dye-sensitized nanocrystalline TiO2 and TiO2/Ta2O5 core-shell photoanodes in aqueous electrolytes using TA spectroscopy, intensity-modulated photovoltage spectroscopy (IMVS), and photoelectrochemical impedance spectroscopy (PEIS). The fast recombination rates measured by TA result from strong laser excitation that leads to high electron occupancy in TiO2, whereas IMVS modulates the concentration of charge-separated states near solar irradiance levels. The recombination processes measured by electrochemical methods such as IMVS, PEIS, and transient photovoltage are the discharging of injected electrons in TiO2, as evidenced by the close agreement between the nearly first-order recombination rates probed by IMVS and the RC time constants derived from PEIS data. However, IMVS measurements at variable probe light intensity reveal that the reaction orders for the recombination of injected electrons with oxidized sensitizer molecules are far from unity. This kinetic analysis is relevant to understanding steady-state recombination rates in full WS-DSPECs in which molecular and nanoparticle catalysts are used to oxidize water.


Asunto(s)
Colorantes/química , Técnicas Electroquímicas , Agua/química , Cinética , Oxidación-Reducción , Procesos Fotoquímicos , Análisis Espectral
10.
Biochim Biophys Acta Mol Basis Dis ; 1864(1): 263-273, 2018 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-29107091

RESUMEN

Alzheimer's disease (AD) is an amyloid-related neurodegenerative disorder and is also considered to be a metabolic disease. Thus, investigation of metabolic mechanisms of amyloid pathology progression is of substantial importance for the diagnosis, prevention and treatment of AD. In the present study, cognitive function and brain metabolism were explored in the transgenic APP/PS1 mouse model of amyloid pathology at different ages. Using an NMR-based metabolomic approach, we examined metabolic changes in six different brain regions of wild-type and APP/PS1 mice at 1, 5 and 10months of age. Learning and memory performance in mice was evaluated using the Morris water maze test. Furthermore, a generalized linear mixed model was employed to analyze the interaction effect between the mouse-type and brain region (or age) on metabolic alterations. Brain region-specific changes in energy metabolism occurred prior to a very early-stage of amyloid pathology (1month of age) in APP/PS1 mice. A hypermetabolic state was identified in the brains of APP/PS1 mice at 5months of age, and the hypothalamus was identified as the main brain region that underwent significant metabolic alterations. The cognitive function of APP/PS1 mice was impaired at 10months of age; moreover, the hypermetabolic state identified in various brain regions at 5months of age was also significantly decreased. In conclusion, our results suggest that a hypothalamic metabolism abnormality may comprise a potential indicator for the early-diagnosis and monitoring of amyloid pathology progression.


Asunto(s)
Enfermedad de Alzheimer/genética , Enfermedad de Alzheimer/patología , Precursor de Proteína beta-Amiloide/genética , Hipotálamo/metabolismo , Hipotálamo/patología , Presenilina-1/genética , Enfermedad de Alzheimer/metabolismo , Precursor de Proteína beta-Amiloide/metabolismo , Amiloidosis/genética , Amiloidosis/metabolismo , Amiloidosis/patología , Animales , Encéfalo/metabolismo , Encéfalo/patología , Encefalopatías Metabólicas/genética , Encefalopatías Metabólicas/metabolismo , Encefalopatías Metabólicas/patología , Cognición/fisiología , Modelos Animales de Enfermedad , Femenino , Masculino , Ratones , Ratones Endogámicos C57BL , Ratones Transgénicos , Presenilina-1/metabolismo
11.
Metab Brain Dis ; 32(2): 585-593, 2017 04.
Artículo en Inglés | MEDLINE | ID: mdl-28070703

RESUMEN

Diabetes mellitus (DM) can result in cognitive dysfunction, but its potential metabolic mechanisms remain unclear. In the present study, we analyzed the metabolite profiling in eight different brain regions of the normal rats and the streptozotocin (STZ)-induced diabetic rats accompanied by cognitive dysfunction using a 1H NMR-based metabolomic approach. A mixed linear model analysis was performed to assess the effects of DM, brain region and their interaction on metabolic changes. We found that different brain regions in rats displayed significant metabolic differences. In addition, the hippocampus was more susceptible to DM compared with other brain regions in rats. More interestingly, significant interaction effects of DM and brain region were observed on alanine, creatine/creatine-phosphate, lactate, succinate, aspartate, glutamate, glutamine, γ-aminobutyric acid, glycine, choline, N-acetylaspartate, myo-inositol and taurine. Based on metabolic pathway analysis, we speculate that cognitive dysfunction in the STZ-induced diabetic rats may be associated with brain region-specific metabolic alterations involving energy metabolism, neurotransmitters, membrane metabolism and osmoregulation.


Asunto(s)
Química Encefálica/efectos de los fármacos , Trastornos del Conocimiento/metabolismo , Trastornos del Conocimiento/psicología , Diabetes Mellitus Experimental/metabolismo , Diabetes Mellitus Experimental/psicología , Espectroscopía de Resonancia Magnética/métodos , Metabolómica/métodos , Animales , Masculino , Aprendizaje por Laberinto/efectos de los fármacos , Redes y Vías Metabólicas , Ratas Sprague-Dawley
12.
Molecules ; 22(9)2017 09 15.
Artículo en Inglés | MEDLINE | ID: mdl-28914810

RESUMEN

Dendrobium officinale Kimura & Migo (D. officinale) is a precious herbal medicine. In this study, we investigated metabolic mechanism underlying the effect of D. officinale water extract (DOWE) on diabetes prevention in mice after streptozotocin (STZ) exposure using NMR-based metabolomics. Interestingly, we found a decrease in blood glucose and an increase in liver glycogen in mice pretreated with DOWE after STZ exposure. The DOWE pretreatment significantly increased citrate and glutamine in the serum as well as creatine, alanine, leucine, isoleucine, valine, glutamine, glutathione and taurine in the liver of STZ-treated mice. Furthermore, serum glucose was significantly negatively correlated with citrate, pyruvate, alanine, isoleucine, histidine and glutamine in the serum as well as alanine and taurine in the liver. These findings suggest that the effect of DOWE on diabetes prevention may be linked to increases in liver glycogen and taurine as well as the up-regulation of energy and amino acid metabolism.


Asunto(s)
Dendrobium/química , Diabetes Mellitus Experimental/tratamiento farmacológico , Extractos Vegetales/química , Animales , Glucemia/metabolismo , Ácido Cítrico/sangre , Hígado/metabolismo , Espectroscopía de Resonancia Magnética , Masculino , Metabolómica , Ratones Endogámicos C57BL , Extractos Vegetales/farmacología , Extractos Vegetales/uso terapéutico , Solubilidad , Agua
13.
J Am Chem Soc ; 138(15): 5143-9, 2016 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-27031870

RESUMEN

The controlled exfoliation of transition metal dichalcogenides (TMDs) into pristine single- or few-layer nanosheets remains a significant barrier to fundamental studies and device applications of TMDs. Here we report a novel strategy for exfoliating crystalline MoS2 into suspensions of nanosheets with retention of the semiconducting 2H phase. The controlled reaction of MoS2 with substoichiometric amounts n-butyllithium results in intercalation of the edges of the crystals, which are then readily exfoliated in a 45 vol % ethanol-water solution. Surprisingly, the resulting colloidal suspension of nanosheets was found (by electron microscopy and atomic force microscopy) to consist mostly of trilayers. The efficiency of exfoliation of the pre-intercalated sample is increased by at least 1 order of magnitude relative to the starting MoS2 microcrystals, with a mass yield of the dispersed nanosheets of 11-15%.

14.
Nano Lett ; 15(9): 5956-60, 2015 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-26288218

RESUMEN

Exfoliated 2H molybdenum disulfide (MoS2) has unique properties and potential applications in a wide range of fields, but corresponding studies have been hampered by the lack of effective routes to it in bulk quantities. This study presents a rapid and efficient route to obtain exfoliated 2H MoS2, which combines fast sonication-assisted lithium intercalation and infrared (IR) laser-induced phase reversion. We found that the complete lithium intercalation of MoS2 with butyllithium could be effected within 1.5 h with the aid of sonication. The 2H to 1T phase transition that occurs during the lithium intercalation could be also reversed by IR laser irradiation with a DVD optical drive.

15.
Nat Commun ; 15(1): 8463, 2024 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-39349448

RESUMEN

The electrocatalytic valorization of polyethylene terephthalate-derived ethylene glycol to valuable glycolic acid offers considerable economic and environmental benefits. However, conventional methods face scalability issues due to rapid activity decay of noble metal electrocatalysts. We demonstrate that a dynamic potential cycling approach, which alternates the electrode potential between oxidizing and reducing values, significantly mitigates surface deactivation of noble metals during electrochemical oxidation of ethylene glycol. This method enhances catalyst activity by 20 times compared to a constant-potential approach, maintaining this performance for up to 60 h with minimal deactivation. In situ Raman and X-ray absorption spectroscopy show that this effectiveness results from efficient removal of surface oxide during the reaction. The strategy is applicable to polyethylene terephthalate hydrolysates and various noble metals, such as palladium, gold, and platinum, with palladium showing a high conversion rate in recent studies. Our approach offers an efficient and durable method for electrochemical upcycling of biomass-derived compounds.

16.
RSC Adv ; 14(37): 26738-26746, 2024 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-39183997

RESUMEN

Alkaline polymer electrolyte fuel cells (APEFCs) have achieved notable advancements in peak power density, yet their durability during long-term operation remains a significant challenge. It has been recognized that increasing the hydrophobicity of the catalyst layer can effectively alleviate the performance degradation. However, a microscopic view of how hydrophobicity contributes to the stability of the catalyst layer microstructure is not clear. Here, we construct a membrane electrode assembly (MEA) with enhanced structural stability and durability by incorporating polytetrafluoroethylene (PTFE) particles into the catalyst layer. MEAs modified by this approach exhibit stabilized voltage platforms in current step tests and reduced hysteresis in current-voltage polarization curves during operation, indicating the critical role of PTFE in the removal of the excess water within the catalyst layer. Fuel cells with PTFE modification show more than 45% increase in electrochemical durability. By characterizing with field-emission scanning electron microscopy (FE-SEM) the surface and the internal microstructures of MEAs after durability tests, we find that the catalyst layers modified by PTFE experience much less reduction in porosity and less agglomeration of the solid components. These findings elucidate the microscopic mechanisms by which hydrophobicity promotes a more stable catalyst layer structure, thereby enhancing the durability of APEFCs. This research advances our understanding of hydrophobicity's impact on catalyst layer stability and offers a practical method to enhance the durability of APEFCs.

17.
Animals (Basel) ; 14(6)2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38540053

RESUMEN

The purpose of this study was to determine the efficacy of tannic acid on the antioxidative function, immunity, and intestinal barrier of broilers co-infected with coccidia and Clostridium perfringens (CCP). A total of 294 1-day-old arbor acres(AA) broilers were divided into three groups: control group (CON), CCP co-infected group (CCP), and 1000 mg/kg TA + CCP co-infected group (CTA). This trial lasted for 28 days. The results showed that the CCP group decreased the activity of glutathione peroxidase (GSH-Px), total superoxide dismutase (T-SOD), catalase (CAT), and total antioxidant capacity (T-AOC) levels and increased the contents of hydrogen peroxide (H2O2) and malondialdehyde (MDA) in the jejunum (p < 0.05). The mRNA levels of GSH-Px3 and CAT in the liver and jejunum, and the mRNA levels of GSH-Px3, SOD, HO-1, and NAD(P)H quinone oxidoreductase I (NQO1) in the liver were down-regulated by CCP challenge (p < 0.05). In addition, the Keap1 and Nrf2 mRNA levels in the liver and jejunum, jejunal glutathione S-transferase (GST), and heme-oxygenase-1 (HO-1) were upregulated in the CCP group compared with CON (p < 0.05). The mRNA levels of interleukin 8 (IL-8), IL-1ß, inducible nitric oxide synthase (iNOS), and interferon γ (IFN-γ) in the jejunum were elevated, and jejunal mRNA levels of IL-10, zonula occludens protein1 (ZO-1), claudin-1, claudin-2, and occludin were decreased in the CCP treatment (p < 0.05). Dietary supplementation with 1000 mg/kg TA increased the activity of GSH-Px, T-SOD, CAT, and T-AOC and decreased the contents of H2O2 and MDA in the jejunum (p < 0.05). Compared with the CCP group, TA decreased the mRNA level of Keap1 and Nrf2 in the liver and jejunum, increased the GSH-Px3, SOD, and CAT mRNA in the liver, and alleviated the rise of IL-8, IL-1ß, iNOS, and IFN-γ and decrease in IL-10, occludin gene expression in the jejunum (p < 0.05). In conclusion, the addition of 1000 mg/kg TA to the diet improved the jejunal barrier, mitigated the jejunal inflammation, and increased the antioxidant capacity of the liver and jejunum through the activation of the transcription factor Nrf2 downstream of the Nrf2-Keap1 pathway in broilers with NE condition.

18.
Nanotechnology ; 24(30): 305401, 2013 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-23818035

RESUMEN

Detailed first-principles computations were performed on the geometric and electronic properties of the interfaces between graphene and ZnO polar surfaces. A notable van der Waals force exists at the interface, and charge transfer occurs between graphene and ZnO as a result of the difference in their work functions. The Dirac point of graphene remains intact despite its adsorption on ZnO, implying that its interaction with ZnO does not affect the superior conductivity of graphene. Excited electrons within the energy range of 0-3 eV (versus Fermi energy) in the hybrid systems are mainly accumulated on graphene. The computations provide a theoretical explanation for the good performance of graphene/ZnO hybrid materials in photocatalysts and solar cells.

19.
Sheng Li Xue Bao ; 65(2): 143-8, 2013 Apr 25.
Artículo en Zh | MEDLINE | ID: mdl-23598869

RESUMEN

One of the major circulatory changes that occur in human during space flight and simulated weightlessness is a cerebral redistribution of body fluids, which is accompanied by an increase of blood volume in the upper body. Therefore, atrial myocardium should increase the secretion of atrial natriuretic peptide (ANP), but the researches lack common conclusion until now. The present study was to investigate the expression level of ANP in simulated weightlessness rats, and to confirm the changes of ANP by observing the associated proteins of soluble N-ethylmaleimide-sensitive factor attachment protein receptors (SNAREs). The tail-suspended rat model was used to simulate weightlessness. Western blots were carried out to examine the expression levels of ANP and SNARE proteins in atrial and left ventricular myocardium. The results showed that ANP expression in atrial myocardium showed an increase in 4-week tail-suspended rats (SUS) compared with that in the synchronous control rats (CON). We only detected a trace amount of ANP in the left ventricular myocardium of the CON, but found an enhanced expression of ANP in left ventricular myocardium of the SUS. Expression of VAMP-1/2 (vesicle associated SNARE) increased significantly in both atrial and left ventricular myocardium in the SUS compared with that in the CON. There was no difference of the expression of syntaxin-4 (target compartment associated SNARE) between the CON and SUS, but the expression of SNAP-23 showed an increase in atrial myocardium of the SUS compared with that in the CON. Synip and Munc-18c as regulators of SNAREs did not show significant difference between the CON and SUS. These results suggest that the expression of ANP shows an increase in atrial and left ventricular myocardium of 4-week tail-suspended rats. Enhanced expression of VAMP-1/2 associated with ANP vesicles confirms the increased expression of ANP in atrial and left ventricular myocardium.


Asunto(s)
Factor Natriurético Atrial/metabolismo , Miocardio/metabolismo , Simulación de Ingravidez , Animales , Ventrículos Cardíacos/metabolismo , Ratas , Proteínas SNARE/metabolismo , Proteína 1 de Membrana Asociada a Vesículas/metabolismo , Proteína 2 de Membrana Asociada a Vesículas/metabolismo
20.
J Hazard Mater ; 453: 131383, 2023 07 05.
Artículo en Inglés | MEDLINE | ID: mdl-37080023

RESUMEN

Recently, the cryogel as a special type of hydrogel was widely used in the field of medicine due to its porous structure and good biocompatibilit. However, great challenges existed for its irregular pore size and incompressible property, limiting its application in other fields. In this study, a novel silk fibroin-based cryogel (named SF@PVA/CS) with regulable pore size, excellent elasticity and durability was constructed using a green dual-directional crosslink strategy. The SF@PVA/CS was prepared by using silk fibroin (SF) as bone scaffold, and chitosan (CS) and polyvinyl alcohol (PVA) as polymer hydrogel which was introduced into the inner bone scaffold of SF. Such a brand-new cryogel possessed three-dimensional dual network structure, which can overcome the shortcoming of unregulatable pore size and incompressibility of traditional cryogel. Additionally, the developed SF@PVA/CS membrane was used for water purification for the first time, which exhibited superior selective permeation, excellent anti-fouling and brilliant self-cleaning property, and it can achieve the purification of both oil/water emulsion and methylene blue solution. This study expanded the application of SF-based cryogel, providing a novel routine for designing new-type composite cryogel and widening the application of dual-directional crosslink strategy developed in this study for facilitating the purification of wastewater.


Asunto(s)
Quitosano , Fibroínas , Purificación del Agua , Fibroínas/química , Criogeles , Quitosano/química , Alcohol Polivinílico/química
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