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1.
Biomed Opt Express ; 15(1): 59-76, 2024 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-38223179

RESUMEN

Hypoxia is a critical tumor microenvironment (TME) component. It significantly impacts tumor growth and metastasis and is known to be a major obstacle for cancer therapy. Integrating hypoxia modulation with imaging-based monitoring represents a promising strategy that holds the potential for enhancing tumor theranostics. Herein, a kind of nanoenzyme Prussian blue (PB) is synthesized as a metal-organic framework (MOF) to load the second near-infrared (NIR-II) small molecule dye IR1061, which could catalyze hydrogen peroxide to produce oxygen and provide a photothermal conversion element for photoacoustic imaging (PAI) and photothermal therapy (PTT). To enhance stability and biocompatibility, silica was used as a coating for an integrated nanoplatform (SPI). SPI was found to relieve the hypoxic nature of the TME effectively, thus suppressing tumor cell migration and downregulating the expression of heat shock protein 70 (HSP70), both of which led to an amplified NIR-II PTT effect in vitro and in vivo, guided by the NIR-II PAI. Furthermore, label-free multi-spectral PAI permitted the real-time evaluation of SPI as a putative tumor treatment. A clinical histological analysis confirmed the amplified treatment effect. Hence, SPI combined with PAI could offer a new approach for tumor diagnosing, treating, and monitoring.

2.
Front Vet Sci ; 10: 1228109, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37576830

RESUMEN

Subgroup K avian leukosis virus (ALV-K) is a new subgroup of avian leukosis virus (ALV) that was first defined in 2012 and has been become prevalent in Chinese native chickens in recent years. An in-depth analysis of the genetic diversity of ALV-K was performed in the study. By Blast analysis, the env gene and the sequences of the 25 ALV-K isolates we isolated were found to be closely related to the isolates from Guangdong, Hebei, Jiangsu, and Hubei provinces, China. Further eighty-nine sequences of the gp85 gene of ALV-K strains available were used in the phylogenetic and genetic distance analyses for the classification. ALV-K was divided into two second-order clades (Clades 1.1 and 1.2) and three third-order clades (Clades 1.2.1, 1.2.2, and 1.2.3), indicating that not only 1.1 and 1.2.3, the two old clades which are prevalent in Japan, but also two new clades (1.2.1, 1.2.2), are co-prevalent in China. The representative strains of each clade were defined for the first time. Notably, Clade 1.2.2 was found to have a deletion of an amino acid residue in the gp85 gene, which was obviously different from Clades 1.1, 1.2.1, and 1.2.3. The proposed classification method will facilitate future studies of ALV-K epidemiology and the comparison of sequences obtained across the world. The first global comprehensive molecular epidemiological analysis was accomplished on the emerging ALV-K.

3.
Quant Imaging Med Surg ; 13(2): 865-877, 2023 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-36819244

RESUMEN

Background: This study developed and validated an ultrasound nomogram based on conventional ultrasound and dual-mode elastography to differentiate breast masses. Methods: The data of 234 patients were collected before they underwent breast mass puncture or surgery at 4 different centers between 2016 and 2021. Patients were divided into 5 datasets: internal validation and development sets from the same hospital, and external validation sets from the 3 other hospitals. In the development cohort, age and 294 different ultrasound and elastography features were obtained from ultrasound images. Univariate logistic regression and least absolute shrinkage and selection operator (LASSO) regression were used for data reduction and visualization. Multivariable logistic regression analysis was used to develop the prediction model and ultrasound nomogram. Receiver operating characteristic (ROC) curve analysis, calibration curves, integrated discrimination improvement, and the net reclassification index were used to evaluate nomogram performance; decision curve analysis (DCA) and clinical impact curves were used to estimate clinical usefulness. Results: In the development cohort, margin, posterior features, shape, vascularity, (the mean shear wave elastography value of 1.5 mm surrounding tissues in a breast mass) divided by (the mean shear wave elastography value of the breast mass)-shell mean/A mean1.5(E), (the ratio of strain elastography of adipose tissue near a breast mass) divided by [the ratio of strain elastography of (the breast mass adds the 1.5 mm surrounding tissues in the breast mass)]-B/A'1.5 were selected as predictors in multivariable logistic regression analysis, comprising Model 1. Among the 5 cohorts, Model 1 performed best, with areas under the curve (AUC) of 0.92, 0.84, 0.87, 0.93, and 0.89, respectively. The AUCs were 0.90, 0.82, 0.83, 0.91, and 0.85, respectively, in Model 2 (margin + posterior features + shape + vascularity) and 0.80, 0.76, 0.77, 0.87, and 0.80, respectively, in Model 3 [shell mean/A mean1.5(E) + B/A'1.5]. Conclusions: Our ultrasound nomograms facilitate exposure to the features and visualization of breast cancer. Shell mean/A mean1.5(E), B/A'1.5 integrated with margin, posterior features, shape, and vascularity are superior at identifying breast cancer, and are worthy of further clinical investigation.

4.
Front Vet Sci ; 9: 901292, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36110503

RESUMEN

Avian hepatitis E virus (HEV) is a major pathogen associated with hepatitis splenomegaly syndrome in chickens and has been reported in China. Phylogenetic trees, Bayesian analysis, positive selection sites screening, and recombination analysis were first used to comprehend the global avian HEVs. All the avian HEV strains, including a new isolate named GX20A1 got from Donglan Black chicken in Guangxi, China, were uniformly defined into four genotypes, and GX20A1, belongs to Genotype 3. The topology of the phylogenetic tree based on the sequences of a 339-bp fragment (coding the helicase) in open reading frame (ORF) 1 of the avian HEVs was consistent with that based on the full-genome sequence. The estimated evolution rate of avian HEVs is 2.73 × 10-3 substitution/site/year (95% confidence interval (CI): 8.01 × 10-4-4.91 × 10-3), and the estimated genetic diversity of the strains experienced a declining phase from 2010 to 2017 and stabilized after 2017. It was further found that the Genotype 3 HEVs, including isolates from Hungary and China, likely originated in the 1930s. Notably, GX20A1 was gathered in the same branch with a Genotype 3 Guangdong isolate CaHEV-GDSZ01, which appeared earlier than GX20A1. In addition, two positive selection sites were identified, one for each of ORF1 and ORF2. Overall, the study revealed that avian HEVs were uniformly defined into four genotypes, and a 339-bp fragment in ORF1 of the viral genome could be used for the classification. A Genotype 3 isolate GX20A1 was first found from Donglan Black chicken and most likely originated from Guangdong.

5.
ACS Appl Mater Interfaces ; 14(34): 38727-38738, 2022 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-35973162

RESUMEN

High-entropy oxides (HEOs) offer unique features through a combination of incompatible metal cations to a single crystalline lattice. Owing to their special characteristics such as abundant cation compositions, high entropy stabilization, chemical and thermal stability, and lattice distortion effect, they have drawn ever-increasing attention for various applications. However, very few studies have been reported for catalytic application, and developing HEOs with large surface areas for efficient catalytic application is still in infancy. Herein, we design nanostructured HEO of (FeNiCoCrCu)3O4 using metal-organic frameworks (MOFs) as sacrificial templates to achieve a large surface area, high density of exposed active sites, and more oxygen vacancies. Single-crystalline phase HEOs with surface area as large as 206 m2 g-1 are produced and further applied as bifunctional electrocatalysts for the urea oxidation reaction (UOR) and oxygen evolution reaction (OER). Benefiting from enhanced oxygen vacancies and a large surface area with abundant exposed active sites, the optimized HEO exhibited excellent electrocatalytic activity toward UOR with a very low potential of 1.35 V at the current density of 10 mA cm-2 and showed long-term stability for 36 h operation, making a significant catalytic performance over previously reported HEOs. Moreover, the HEO demonstrated an efficient catalytic performance toward OER with a low overpotential of 270 mV at 10 mA cm-2 and low Tafel slope of 49 mV dec-1. The excellent catalytic activity is ascribed to the starting MOF precursor and favorable high-entropy effect.

6.
Artículo en Inglés | MEDLINE | ID: mdl-35162687

RESUMEN

There is evidence that the built environment has an influence on street vitality. However, previous studies seldom assess the direct, indirect, and total effect of multiple environmental elements at the city level. In this study, the features of the street vitality on Xiamen Island are described based on the location-based service Big Data. Xiamen Island is the central urban area of Xiamen, one of the national central cities in China. With the help of multi-source data such as street view images, the condition of design that is difficult to effectively measure with traditional data can be better explored in detail on a macro scale. The built environment is measured through a 5D system at the city level, including Density, Diversity, Design, Destination accessibility, and Distance to transit. Spatial panel Durbin models are constructed to analyze the influence of the built environment on the street vitality on weekdays and weekends, and the direct, indirect, and total effects are evaluated. Results indicate that at the city level, the built environment plays a significant role in promoting street vitality. Functional density is not statistically significant. Most of the elements have spatial effects, except for several indicators in the condition of the design. Compared with the conclusions of previous studies, some indicators have different effects on different spatial scales. For instance, on the micro scale, greening can enhance the attractiveness of streets. However, on the macro scale, too much greening brings fewer functions along the street, which inhibits the street vitality. The condition of design has the greatest effect, followed by destination accessibility. The differences in the influences of weekdays and weekends are mainly caused by commuting behaviors. Most of the built environment elements have stronger effects on weekends, indicating that people interact with the environment more easily during this period.


Asunto(s)
Entorno Construido , Urbanización , Ciudades , Investigación Empírica , Planificación Ambiental , Humanos , Características de la Residencia , Transportes
7.
Talanta ; 233: 122469, 2021 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-34215104

RESUMEN

Folic acid (FA) is the natural form of water-soluble vitamins widely found in most plants and animal products and its deficiency leads to several human body abnormalities. The advancements of metal nanoclusters are highly increasing due to their molecule-like optical properties and attractive applications. Because of increasingly demand of noble metal nanoclusters as sensing templates, different synthesis methods have been developed for facile synthesis of noble metal nanoclusters. Herein, red-emitting fluorescent bovine serum albumin (BSA)-capped Au-Ag bimetallic NCs are facilely synthesized through green one-pot synthetic approach. The effect of silver on the fluorescence properties of Au NCs was investigated and it was found that introduction of silver can enhance the fluorescence intensity. The fluorescence intensity of the as-prepared Au-Ag nanoclusters gets quenched in the presence of folic acid in an aqueous medium and it was used as ultrasensitive sensing probe for FA detection. The developed Au-Ag NCs-based sensing probe shows linear response in the wide range of 0-100 µM and the detection limit is as low as 0.47 nM. Its applicability has also been confirmed successfully in real human serum, urine and FA tablet samples. Due to the high stability, sensitivity and selectivity, the developed bimetallic cluster sensing system is highly promising to be applied in the pharmaceutical and clinical laboratories.


Asunto(s)
Nanopartículas del Metal , Plata , Animales , Ácido Fólico , Oro , Humanos , Albúmina Sérica Bovina , Espectrometría de Fluorescencia
8.
ACS Appl Mater Interfaces ; 13(22): 25937-25945, 2021 Jun 09.
Artículo en Inglés | MEDLINE | ID: mdl-34041911

RESUMEN

Electrochemical conversion of CO2 into valuable products is a promising approach. Efficient electrocatalysts are highly desirable but remain to be developed. Here, we proposed a molecular encapsulation strategy to enrich intermediates for facilitating electrochemical conversion of CO2 to C2H4. This strategy is combining M-TCPP [M = FeCl, Co, and Ni; TCPP = tetrakis(4-carboxyphenyl) porphyrin] with a Cu-based metal-organic framework (Cu-MOF) to create a series of metalloporphyrin-decorated Cu catalysts with a coral-like shape (named as M-TCPP@Cu). M-TCPP in the catalysts could supply more CO intermediates to the Cu sites, giving high selectivity for producing C2H4 and lowering overpotentials for CO2 reduction. Meanwhile, the coral-like structure of the catalyst with abundant active sites is conducive to mass diffusion and benefits the conversion of CO2. We realized a higher C2H4 Faradaic efficiency (FE) of 33.42% at -1.17 V versus reversible hydrogen electrode (RHE) on the Fe-TCPP@Cu electrode than that on the sole Cu electrode (16.85%, at -1.27 V vs RHE). Furthermore, due to the encapsulated structure resulted from one-pot reaction that ensures the dispersion of active centers in M-TCPP, metalloporphyrin-decorated Cu catalysts show better performance than the physical mixture of Cu-MOFs and M-TPPs (M = FeCl, Co, and Ni; TPP = 5,10,15,20-tetraphenylporphyrin). The results provide a new strategy for the design of high-performance Cu catalysts from Cu-MOFs for CO2 conversion.

9.
Anal Chem ; 93(20): 7465-7472, 2021 May 25.
Artículo en Inglés | MEDLINE | ID: mdl-33973779

RESUMEN

Metal oxide semiconductors (MOS) with different nanostructures have been widely used as gas sensing materials due to the tunable interface structures and properties. However, further improvement of the sensing sensitivity and selectivity is still challenging in this area. Constructing appropriate heterogeneous interface structures and oxygen vacancies is one of the important strategies to tune the sensing properties of MOS. In the present study, interfacial heterostructures in PdxW18O49 nanowires (PdxW18O49 NWs) were fabricated and manipulated by doping different Pd contents through a simple hydrothermal process. Relevant characterization proved that the structure and composition of the one-dimensional (1D) nanomaterial can be effectively changed by Pd doping. It was found that the oxygen vacancy concentration increases first with the increase of Pd content, and when the Pd content increases to 7.18% (Pd7.18%W18O49 NWs), the oxygen vacancy content reaches the maximum (52.5%). If the Pd content continues to increase, the oxygen vacancy ratio decreases. The gas sensing investigations illustrated that the PdxW18O49 NWs exhibited enhanced sensing properties than pure W18O49 NWs toward acetone. Among the as-prepared catalysts, the Pd7.18%W18O49 NWs showed the best sensing response and the fastest response-recovery speeds (5 and 10 s, respectively) at a working temperature of 175 °C. In addition, this 1D nanostructure with fabricated heterostructures also delivers a good sensing selectivity and a wide detection range from 100 ppb to 300 ppm, with maintaining excellent performance in the presence of high concentrations of ethanol and carbon dioxide. The excellent gas sensing behavior could be attributed to the generated oxygen vacancies and the heterostructures upon Pd doping. This study offers a novel strategy for the design of high-performance gas sensors for ppb-level acetone sensing.

10.
J Colloid Interface Sci ; 590: 518-526, 2021 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-33578239

RESUMEN

Photocatalytic degradation of organic dyes by sunlight can greatly simplify the catalytic devices and save the cost. The development of photocatalysts for organic pollutants degradation driven by sunlight at room temperature still faces serious challenges. In this work, we developed a novel Pd-W18O49 nanowire photocatalyst for high efficiency, high stability, and sunlight-induced degradation of methylene blue and neutral red. It was found that after Pd introducing, the band gap energy of W18O49 nanowires lowers from 2.77 to 2.44 eV, which can accelerate the electron jump from the valence band to the conduction band, resulting in the efficient separation of electrons and holes. Meanwhile, with Pd introducing to the W18O49 nanowires, interfacial heterojunction with the Schottky barrier is formed, which can reduce the rate of electron-hole recombination. The catalytic results show that the obtained Pd-W18O49 nanowires demonstrate enhanced photodegradation capacity in comparison with W18O49 nanowires. Especially, with Pd-W18O49 nanowires (10 mg) as photocatalyst, 98.4% of methylene blue and 96.1% of neutral red can be decomposed within 40 min under sunlight irradiation. Besides, the photocatalytic degradation pathways of methylene blue and neutral red on the Pd-W18O49 nanowires are also proposed. This study provides a good strategy for the design and preparation of highly efficient 1D heterojunction-based photocatalysts for the degradation of environmental organic pollutants.

11.
Chem Commun (Camb) ; 57(16): 2033-2036, 2021 Feb 25.
Artículo en Inglés | MEDLINE | ID: mdl-33506835

RESUMEN

Iron porphyrin and carbon black (CB) were utilized to fabricate an iron-nitrogen doped carbon (Fe-N-C) catalyst to create a new heterogeneous catalytic system with CdS to drive CO2 reduction to CO under UV/vis light (AM 1.5G) irradiation. The system delivers a high CO production yield of 111 mmol gcat-1 and a large turnover number (TON) of 1.22 × 103 in 8 h with a selectivity of 85%, all of which are competitive with state-of-the-art systems. The mechanism of the system was investigated by experimental and theoretical methods indicating that the high affinity between the iron active center and the *COOH intermediate facilitates the brilliant catalytic performance. This work provides a new direction for constructing heterogeneous CO2 photoreduction systems.

12.
Anal Bioanal Chem ; 413(6): 1639-1649, 2021 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-33483839

RESUMEN

Balanced level of hemin in the body is fundamentally important for normal human organ function. Therefore, environmentally benign, stable, and fluorescent metal nanoclusters (NCs) for selective and sensitive detection of hemin have been investigated and reported. Herein, highly orange red emissive gold NCs are successfully synthesized using glutathione as a reducing and stabilizing agent (GSH-Au NCs). The clusters are characterized using various techniques like Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), UV-vis spectroscopy, and fluorescence spectrometer. The fluorescence intensity of as-synthesized Au NCs strongly quenched upon addition of different concentrations of hemin. The decrease in fluorescence intensity of GSH-Au NCs has been applied for determination of hemin concentration in the linear range from 1 to 25 nM with a low limit of detection (LOD) of 0.43 nM. The method was also successfully applied for quantification of hemin in human serum sample. In view of this reality, the system can be considered as a possible strategy and excellent platform for determination of hemin in various areas of application.


Asunto(s)
Colorantes Fluorescentes/análisis , Oro/química , Hemina/análisis , Hemina/química , Nanopartículas del Metal/química , Técnicas Biosensibles/métodos , Glutatión/química , Humanos , Límite de Detección , Microscopía Electrónica de Transmisión , Espectrometría de Fluorescencia , Espectrofotometría Ultravioleta , Espectroscopía Infrarroja por Transformada de Fourier , Resonancia por Plasmón de Superficie , Temperatura
13.
Dalton Trans ; 50(1): 384-390, 2021 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-33320135

RESUMEN

Metal-organic frameworks (MOFs) represent an emerging class of platforms to assemble single site photocatalysts for artificial photosynthesis. In this work, we report a new CO2 reduction photocatalyst (UiO-68-Fe-bpy) based on a robust Zr(iv)-MOF platform with incorporated Fe(bpy)Cl3 (bpy refers to the 4'-methyl-[2,2'-bipyridine] moiety) via amine-aldehyde condensation. We show that this hybrid catalyst can reduce CO2 to form CO under visible light illumination with excellent selectivity and enhanced activity with respect to its parent MOF and corresponding homogeneous counterpart. Using steady state and transient absorption (TA) spectroscopy, we show that the enhanced photocatalytic activity of UiO-68-Fe-bpy is attributed to the elongated excited state lifetime of Fe(bpy)Cl3 after being incorporated to the UiO-68-NH2 platform. This work demonstrates the great potential of MOFs as a next generation platform for solar fuel conversion.

14.
Curr Pharm Biotechnol ; 22(10): 1380-1391, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-33238839

RESUMEN

BACKGROUND: Cistanche tubulosa is a tonic in traditional Chinese medicines and has a broad spectrum of biological activity, including anti-inflammatory. However, the anti-inflammatory major constituents of C. tubulosa and their underlying mechanisms are still unknown. OBJECTIVE: The aim of the current study was to explore the separation and structural characterization of lignan glycosides from C. tubulosa (Schenk) Wight., their anti-inflammatory activity and the underlying mechanism. MATERIALS AND METHODS: Fractionation and isolation of the 85% EtOH extract of C. tubulosa (Schenk) Wight. were carried out and the primary ingredients lignan glycosides (1-6) were structurally characterized. CCK8 methods were used to evaluate the cytotoxic effect of lignan glycosides (1-6). Effects of lignan glycosides (1-6) on NO production in LPS/IFN-γ-induced RAW264.7 macrophages cells were measured using Griess reagent by reaction with nitrite. The mRNA expression levels of iNOS, COX-2, IL-1ß, IL-6, TNF-a, and TGF-ß treated RAW264.7 cells with various concentrations (0, 25 and 50 µg/ml) of lignan glycosides (1, 4) in the presence of LPS (10 ng/ml) and IFN-γ (20 ng/ml) for 24 h were analyzed by quantitative RT-PCR. Also, the protein expressions of iNOS, COX-2, PI3K, AKT, p-AKT and ß -actin were determined using Western blot analysis. A molecular docking study was performed to investigate the interactions between the lignan glycosides and the PI3K using Autodock vina 1.1.2 package. RESULTS: Six lignan glycosides (1-6) were isolated from stems of C. tubulosa. Among them, (+)- pinoresinol-4-O-ß-D-glucopyranosyl-(1→6)-ß-D-glucopyranoside (5) and eleutheroside E (6) were firstly isolated from C. tubulosa. Of these lignans, 1 and 4 exhibited pronounced inhibitions on NO production with the values of 33.63 ± 4.78 and 39.28 ± 5.52 % at 50 µg/ml, respectively. Additionally, LPS/IFN-γ-induced expression of inducible Nitric Oxide Synthase (iNOS), Cyclooxygenase-2 (COX-2), Interleukin-1ß (IL-1ß), IL-6, and Tumor Necrosis Factor-a (TNF-a) was significantly suppressed by pre-treatment of 1 and 4 in a dose-dependent manner. While 1 and 4 increased the mRNA levels of anti-inflammatory cytokines (TGF-ß). Furthermore, 1 and 4 significantly inhibited the protein levels of PI3K and p-AKT in a dose-dependent manner. CONCLUSION: Taken together, these results suggest that 1 and 4 play an important role in the attenuation of LPS/IFN-γ-induced inflammatory responses in RAW264.7 cells and that the mechanisms involve down-regulation of the PI3K/AKT pathway.


Asunto(s)
Cistanche , Lignanos , Animales , Antiinflamatorios/farmacología , Cistanche/metabolismo , Glicósidos/farmacología , Lignanos/farmacología , Lipopolisacáridos , Macrófagos/metabolismo , Ratones , Simulación del Acoplamiento Molecular , FN-kappa B/metabolismo , Óxido Nítrico/metabolismo , Óxido Nítrico Sintasa de Tipo II , Fosfatidilinositol 3-Quinasas/metabolismo , Proteínas Proto-Oncogénicas c-akt/metabolismo , Células RAW 264.7
15.
ACS Appl Mater Interfaces ; 12(36): 40194-40203, 2020 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-32805843

RESUMEN

Energy-efficient, low-cost, and highly durable catalysts for the electrochemical hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) are extremely important for related sustainable energy systems. In the present work, hierarchical coassembled cobalt molybdenum sulfide nanosheets deposited on carbon cloth (CC) were synthesized as catalysts for hydrogen evolution and urea oxidation. By adjusting the doping amount of Mo, 2D nanosheets with different morphologies and compositions (CoxMoyS-CC) can be obtained. The as-prepared nanosheet materials with abundant active sites exhibit superior properties on the electrochemical HER and UOR in alkaline medium. Significantly, the Mo-doping concentration and composition of the formed nanosheets have large effects on the electrocatalytic activity. The fabricated nanosheets with optimal Mo doping (Co3Mo1S-CC) illustrate the best catalytic properties for the HER in N2-saturated 1.0 M KOH. A small overpotential (85 mV) is needed to meet the current density of 10 mA/cm2. This study indicates that the doping of an appropriate amount of molybdenum into CoS2 nanosheets can efficiently improve the catalytic performance. Also, the nanosheet catalyst exhibits an extremely high electrocatalytic activity for the UOR, and the electrochemical results indicate that a relatively low cell voltage of 1.50 V is needed to obtain the current density of 10 mA/cm2. The present work demonstrates the potential application of CoMoS nanosheets in the energy electrocatalysis area and the insights into performance-boosting through heteroatom doping and optimization of the composition and structure.

16.
Chem Commun (Camb) ; 56(29): 4110-4113, 2020 Apr 14.
Artículo en Inglés | MEDLINE | ID: mdl-32163077

RESUMEN

A new ligand H2L with pyridine and salen moieties and its coordination polymers (CPs) [Mn(L)Cl]·DMF (1) and [Fe(L)Cl]·DMF (2) were synthesized and their photocatalytic activity for the conversion of CO2 into CO under visible-light irradiation was investigated. This is the first instance of pyridyl-salen-ligand based CPs for photocatalyzing CO2 reduction.

17.
Inorg Chem ; 58(13): 8517-8524, 2019 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-31184876

RESUMEN

It is deemed as a desired approach to utilize solar energy for the conversion of CO2 into valuable products, and the majority of the MOFs-based photocatalytic reductions of CO2 have focused on formic acid (HCOOH) production with an organic solvent as the reaction medium. Herein, we report a solvent-free reaction route for the photoreduction of CO2 catalyzed by Fe-MOFs, namely, NH2-MIL-53(Fe) [(Fe(OH)(NH2-BDC)]•G, NH2-MIL-88B(Fe) [Fe3O(H2O)3(NH2-BDC)3]Cl•G, and NH2-MIL-101(Fe) [Fe3O(H2O)3(NH2-BDC)3]Cl•G (NH2-BDC = 2-aminoterephthalic acid; G = guest and/or solvent molecules). Compared with the orthodox reaction route, the present out-of-the-way photocatalytic reduction of CO2 with superior selectivity to CO occurs at the gas-solid interface. The reaction procedure is environmentally friendly and provides a possibility to address the CO2 emission problem. Importantly, NH2-MIL-101(Fe) shows the highest photocatalytic activity among these Fe-MOFs due to its efficient charge separation and electron transfer.

18.
Chem Sci ; 10(18): 4834-4838, 2019 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-31160958

RESUMEN

Facet-dependent catalytic activity of hard materials such as metals and metal oxides is well recognized in previous works. However, it has rarely been established for metal-organic frameworks (MOFs), possibly because the soft crystals of MOFs are conceptually different from the hard solids. In this work, the surface structure of the MOF NH2-MIL-125(Ti) has been investigated by density functional theory (DFT) calculations for the first time. These calculations predict that the {110} facet has a surface energy of 1.18 J m-2, which is superior to those of the {001}, {100} and {111} facets. This difference can be attributed to the larger percentage of exposed metal clusters, which can act as active sites in catalysis. Thus, we have devised and successfully obtained a series of nanoscaled NH2-MIL-125(Ti) MOFs with controlled facets both experimentally and theoretically. The sample containing the {110} facet exhibits the highest photocatalytic hydrogen production activity and apparent quantum yield, which are approximately three times those of the sample with a dominant {111} facet.

19.
Inorg Chem ; 57(5): 2695-2704, 2018 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-29446625

RESUMEN

A combination of carbon dioxide (CO2) capture and chemical fixation in a one-step process is attractive for chemists and environmentalists. In this work, by incorporating chelating multiamine sites to enhance the binding affinity toward CO2, two novel metal-organic frameworks (MOFs) [Zn2(L)(2,6-NDC)2(H2O)]·1.5DMF·2H2O (1) and [Cd2(L)(2,6-NDC)2]·1.5DMF·2H2O (2) (L = N1-(4-(1 H-1,2,4-triazole-1-yl)benzyl)- N1-(2-aminoethyl)ethane-1,2-diamine, 2,6-H2NDC = 2,6-naphthalenedicarboxylic acid, DMF = N, N-dimethylformamide) were achieved under solvothermal conditions. Both 1 and 2 possess high selectivity for adsorption of CO2 over CH4 at room temperature under atmospheric pressure. Moreover, 1 has one-dimensional tubular channels decorated with multiactive sites including NH2 groups and coordination unsaturated Lewis acid metal sites, leading to efficient catalytic activity for chemical fixation of CO2 by reaction with epoxides to give cyclic carbonates under mild conditions.

20.
Zhong Nan Da Xue Xue Bao Yi Xue Ban ; 38(7): 743-7, 2013 Jul.
Artículo en Chino | MEDLINE | ID: mdl-23908090

RESUMEN

OBJECTIVE: To investigate the value of B ultrasonography in the early diagnosis of transient synovitis of hip (TSH) in dogs, and provide the valid base and data for the clinic early diagnosis of TSH. METHODS: Eighty 2-3 month old dogs were injected 0.2% noradrenalin (NA) into the hip joint induced TSH. We observed 5 assessments that included the 99mTC-MDP triphasic imaging, X ray, B ultrasonography, the synovial fluid and the pathological tissue check in different time. RESULTS: Early course of TSH presented the synovium of joint hemangiectasis, hyperaemia, synovium villus hyperplasia, edema, and joint inflammatory exudation. The ischemia of local blood supply of the femoral head was observed by 99mTC-MDP triphasic imaging. Ultrasonography showed the broadening of the anterior space of the hip, but the X ray showed no valid changes. CONCLUSION: B ultrasonography can report the early changes of TSH and may be used in the early diagnosis of TSH in children.


Asunto(s)
Articulación de la Cadera/diagnóstico por imagen , Sinovitis/diagnóstico por imagen , Animales , Perros , Diagnóstico Precoz , Femenino , Articulación de la Cadera/patología , Masculino , Norepinefrina , Sinovitis/inducido químicamente , Sinovitis/patología , Ultrasonografía
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