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Heterostructures and the introduction of heterogeneous elements have been regarded as effective strategies to promote electrochemical performance. Herein, sulfur species are introduced by a simple hydrothermal vulcanization method, which constructs the open heterostructure Fe7S8/Mn(OH)2 as a bifunctional material. The open cordyceps-like morphology can make the material contact more sufficiently with the electrolyte, exposing a large number of reaction sites. Furthermore, the introduction of the heterogeneous element S successfully constructs a heterogeneous interface, the interface-modulated composite material consists of Mn atoms contributing the main density of states (DOS) near the Fermi energy level from the density functional theory (DFT) calculations, which optimizes the adsorption energy of oxygen-containing intermediates during the oxygen evolution reaction (OER) process and reduces the reaction energy barrier, being conducive to the improvement of the material's electrochemical properties. As predicted, the Fe7S8/Mn(OH)2 material exhibits remarkable electrochemical properties, such as an overpotential of 202 mV at 10 mA cm-2 for the oxygen evolution reaction and even a specific capacitance of 2198 F g-1 at 1 A g-1. This work provides new insights into the role of introducing sulfur species and controlling the structure of the material, and exemplifies novel design ideas for developing bifunctional materials for energy storage and conversion.
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Eu3+-induced polystyrene-co-poly(acrylic acid) aggregates (EIPAs) were synthesized using a self-assembly approach, and their structures and photophysical characteristics were examined to achieve effective monochromatic red emission in polymer light-emitting diodes (PLEDs). By adjusting the monomer ratio in RAFT polymerization, the size of Eu3+-induced block copolymer nanoaggregates can be regulated, thereby modulating the luminescence intensity. High-performance bilayer polymer light-emitting devices were fabricated using poly(9,9-dioctylfluorene) (PFO) and 2-(tert-butylphenyl)-5-biphenylyl-1,3,4-oxadiazole (PBD) as the host matrix, with EIPAs as the guest dopant. The devices exhibited narrow red emission at 615 nm with a full width at half-maximum (fwhm) of 15 nm across doping concentrations of 1, 3, 5, and 10 wt %. At a doping concentration of 3 wt %, the device achieved a maximum brightness of 1864.48 cd/m2 at 193.82 mA/cm2 and an external quantum efficiency of 3.20% at a current density of 3.5 mA/cm2. These results indicate that incorporating polystyrene-co-poly(acrylic acid) with Eu3+ complexes enhances the excitation and emission intensity, as well as the structural stability of the emitting layer in PLEDs, thereby improving the device performance.
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Background: The protective role of gut microbiota and its metabolites against intestinal damage in sepsis patients remain unclear. Methods: Fecal samples were acquired from patients categorized into sepsis and non-sepsis groups for analysis of microbial composition via 16S rRNA sequencing and untargeted metabolomics analysis. We assessed the impact of gut microbiota from sepsis patients on intestinal barriers in antibiotic-treated mice. Furthermore, We conducted spearman's correlation analysis to examine the relationship between metabolites and the severity of sepsis. Additionally, we performed animal experiments to validate the functionality of identified metabolites. Results: The diversity of intestinal flora is decreased in patients with sepsis compared to the control group. Through fecal microbiota transplantation experiments, it was discovered that the gut microbiota derived from sepsis patients could induce intestinal damage in antibiotic-treated mice. Metabolomics analysis of the microbiota revealed a significant enrichment of the Valine, leucine, and isoleucine biosynthesis pathway. Further analysis showed a significant decrease in the abundance of L-valine in sepsis patients, which was negatively correlated with APACHE-II and SOFA scores. In sepsis mouse experiments, it was found that L-valine could alleviate sepsis-induced intestinal damage. Conclusion: Alterations in microbial and metabolic features in the gut can affect the severity of sepsis. Furthermore, L-valine can protect against sepsis-induced intestinal injury.
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Microbioma Gastrointestinal , Sepse , Valina , Microbioma Gastrointestinal/efeitos dos fármacos , Sepse/microbiologia , Animais , Camundongos , Humanos , Valina/farmacologia , Valina/uso terapêutico , Masculino , Feminino , Pessoa de Meia-Idade , Transplante de Microbiota Fecal , Índice de Gravidade de Doença , Metabolômica/métodos , Idoso , Fezes/microbiologia , Modelos Animais de Doenças , Camundongos Endogâmicos C57BL , Mucosa Intestinal/metabolismo , Mucosa Intestinal/microbiologia , Intestinos/microbiologia , RNA Ribossômico 16S/genéticaRESUMO
Small-size gold nanoparticles (AuNPs) are showing large potential in various fields, such as photothermal conversion, sensing, and medicine. However, current synthesis methods generally yield lower, resulting in a high cost. Here, we report a novel uni-micelle method for the controlled synthesis of monodisperse gold nanocrystals, in which there is only one kind micelle containing aqueous solution of reductant while the dual soluble Au (III) precursor is dissolved in oil phase. Our synthesis includes the reversible phase transfer of Au (III) and "uni-micelle" synthesis, employing a Au (III)-OA complex as an oil-soluble precursor. Size-controlled monodisperse AuNPs with a size of 4-11 nm are synthesized by tuning the size of the micelles, in which oleylamine (OA) is adsorbed on the shell of micelles and enhances the rigidity of the micelles, depressing micellar coalescence. Monodisperse AuNPs can be obtained through a one-time separation process with a higher yield of 61%. This method also offers a promising way for the controlled synthesis of small-size alloy nanoparticles and semiconductor heterojunction quantum dots.
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Obtaining lignin-based graphite-like microcrystallites at a relatively low carbonization temperature is still very challenging. In this work, we report a new method based on condensed structures, for regulating graphite-like microcrystalline structures via the incorporation of 4,4'-diphenylmethane diisocyanate (MDI) into the main structure of lignin. The effects of MDI on the thermal properties of lignin and the graphite-like microcrystalline structure of lignin-based ultrafine carbon fibers were extensively studied and investigated. The incorporation of MDI decreased the thermal stability of lignin, increased the carbon yield and enhanced the formation of graphite-like microcrystallites, which are beneficial for reducing energy consumption during the preparation of lignin-based carbon fibers. The modified lignin-based ultrafine carbon fibers (M-LCFs) demonstrated satisfactory electrochemical performance, including high specific capacitance, low charge transfer resistance, and good cycle performance. The M-LCFs-3/2 electrode had a specific capacitance of 241.3â¯Fâ¯g-1 at a current density of 0.5 A g-1, and a residual ratio of 90.2â¯% after 2000 charge and discharge cycles. This study provides a new approach to control the graphite-like microcrystalline structure and electrochemical performance while also optimizing the temperature.
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Fibra de Carbono , Grafite , Lignina , Lignina/química , Grafite/química , Fibra de Carbono/química , Cristalização , Temperatura , Capacitância Elétrica , Eletrodos , Carbono/químicaRESUMO
Invasive candidiasis may be caused by Candida albicans (C. albicans) colonization of the intestinal tract. Preventing intestinal damage caused by Candida albicans infection and protecting intestinal barrier function have become a critical issue. Integrated analyses of the microbiome with metabolome revealed a remarkable shift of the gut microbiota and tryptophan metabolites, kynurenic acid (KynA), and indolacrylic acid (IA) in mice infected with C. albicans. The transcriptome sequencing indicated that differentially expressed genes were significantly associated with innate immune responses and inflammatory responses. The results of this study suggest that KynA and IA (KI) can alleviate intestinal damage caused by Candida albicans infection in mice by reducing intestinal permeability, increasing intestinal firmness, alleviating intestinal inflammation, and reducing the secretion of interleukin-22 (IL-22) in the 3 groups of colon innate lymphoid cells (ILC3). We performed a fecal microbiota transplantation (FMT) experiment and found that the intestinal barrier function, inflammation, and IL-22 secretion of ILC3 in the colon lamina propria of the recipient mice subjected to C. albicans infection and KI treatment were consistent with the trends of the donor mice. Our results suggest that tryptophan metabolites may directly regulate colon lamina ILC3 to promote intestinal resistance to C. albicans invasion, or indirectly regulate the ILC3 secretion of IL-22 to play a protective role in the intestinal barrier by affecting intestinal microorganisms, which may become a potential target for alleviating intestine borne C. albicans infection.
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Candida albicans , Candidíase , Colo , Microbioma Gastrointestinal , Interleucina 22 , Interleucinas , Mucosa Intestinal , Triptofano , Animais , Microbioma Gastrointestinal/efeitos dos fármacos , Triptofano/metabolismo , Camundongos , Interleucinas/metabolismo , Candidíase/imunologia , Candidíase/microbiologia , Mucosa Intestinal/metabolismo , Mucosa Intestinal/imunologia , Colo/microbiologia , Colo/imunologia , Colo/metabolismo , Masculino , Linfócitos/imunologia , Linfócitos/metabolismo , Camundongos Endogâmicos C57BL , Imunidade Inata , Transplante de Microbiota FecalRESUMO
ZnO quantum dots (QDs) supported on porous nitrogen-doped carbon (ZnOQDs/P-NC) exhibited excellent electrochemical performance for the electroreduction of CO2 to CO with a faradaic efficiency of 95.3% and a current density of 21.6 mA cm-2 at -2.2 V vs. Ag/Ag+.
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The development of indium phosphide (InP)-based quantum dots (QDs) with a near-infrared (NIR) emission area still lags behind the visible wavelength region and remains problematic. This study describes a one-step in situ pseudohalogen ammonium salt-assisted approach to generate NIR-emitted InP-based QDs with high photoluminescence quantum yields (PLQYs). The coexistence of NH4+ and PF6- ions from NH4PF6 may in situ synchronously etch and passivate the surface oxides and impede the creation of traps under the whole growth process of InP QDs. Experimental findings demonstrated that the in situ pseudohalogen ammonium salt-assisted syntheses technique may feature emission at a full width at half-maximum (fwhm) peak as fine as â¼45 nm and broaden the emission range to around â¼780 nm. A two-step approach for ZnS shells was developed to further improve the PLQY of NIR-emitted InP QDs. Furthermore, the constructed high-power intrinsically stretchable NIR color-conversion film employing the InP-based QDs/polymer composites presented excellent luminescence conversion ability and stretchability.
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Acquiring the ideal blend morphology of the active layer to optimize charge separation and collection is a constant goal of polymer solar cells (PSCs). In this paper, the ternary strategy and the sequential deposition process were combined to make sufficient use of the solar spectrum, optimize the energy-level structure, regulate the vertical phase separation morphology, and ultimately enhance the power conversion efficiency (PCE) and stability of the PSCs. Specifically, the donor and acceptor illustrated a gradient-blended distribution in the sequential deposition-processed films, thus resulting in facilitated carrier characteristics in the gradient-blended devices. Consequently, the PSCs based on D18-Cl/Y6:ZY-4Cl have achieved a device efficiency of over 18% with the synergetic improvement of open-circuit voltage (VOC), short-circuit current density (JSC), and fill factor (FF). Therefore, this work reveals a facile approach to fabricating PSCs with improved performance and stability.
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Indium phosphide (InP) quantum dots (QDs) have become the most recognized prospect to be less-toxic surrogates for Cd-based optoelectronic systems. Due to the particularly dangling bonds (DBs) and the undesirable oxides, the photoluminescence performance and stability of InP QDs remain to be improved. Previous investigations largely focus on eliminating P-DBs and resultant surface oxidation states; however, little attention has been paid to the adverse effects of the surface In-DBs on InP QDs. This work demonstrates a facile one-step surface peeling and passivation treatment method for both In- and P-DBs for InP QDs. Meanwhile, the surface treatment may also effectively support the encapsulation of the ZnSe shell. Finally, the generated InP/ZnSe QDs display a narrower full width at half-maximum (fwhm) of â¼48 nm, higher photoluminescence quantum yields (PLQYs) of â¼70%, and superior stability. This work enlarges the surface chemistry engineering consideration of InP QDs and considerably promotes the development of efficient and stable optoelectronic devices.
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Imunoterapia , Neoplasias , Humanos , Microambiente Tumoral , Neoplasias/terapia , Neoplasias/patologiaRESUMO
BACKGROUND: Complex pathophysiological the specific mechanism of sepsis on CD4+ T-cell responses is less well understood. IL1 receptor accessory protein (IL1RAP) was found to be involved in activating host immune responses. METHOD: Cecum ligation and puncture (CLP) was utilized to build a mouse sepsis model. The experiment was randomly divided into four groups: Sham, CLP, CLP + shNC, and CLP + shIL1RAP group. RESULTS: qRT-PCR suggested mRNA levels of IL1RAP were decreased when IL1RAP was knocked down with the mRNA levels of IL-1ß, NF-κB, and p38 decreased. Histopathology showed severe pathological damage with alveolar integrity lost, red blood cells in the alveoli, massive inflammatory cell infiltration, and the alveolar wall was thickening in the CLP group. The inflammatory cytokine levels of TNF-α, IL-1ß, and IFN-γ were elevated in CLP mice by ELISA. The counts of CD4+ T cells were decreased in sepsis mice in peripheral blood, spleen, and BALF by flow cytometry. However, the above was blocked down when using shIL1RAP. Western blot suggested sh IL1RAP inhibited IL-1ß, NF-κB, and p38 protein expressions. CONCLUSIONS: We defined IL1RAP as a new target gene through NF-κB/MAPK pathways regulating CD4+ T lymphocyte differentiation mediated the progression of sepsis, which is potentially exploitable for immunotherapy.
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Linfócitos T CD4-Positivos , Diferenciação Celular , Modelos Animais de Doenças , NF-kappa B , Sepse , Baço , Animais , Feminino , Masculino , Camundongos , Linfócitos T CD4-Positivos/imunologia , Citocinas/metabolismo , Pulmão/patologia , Pulmão/imunologia , Lesão Pulmonar/imunologia , Lesão Pulmonar/etiologia , Lesão Pulmonar/patologia , Camundongos Endogâmicos C57BL , NF-kappa B/metabolismo , Proteínas Quinases p38 Ativadas por Mitógeno/metabolismo , Sepse/imunologia , Sepse/complicações , Transdução de Sinais , Baço/imunologia , Baço/patologia , Baço/metabolismoRESUMO
Nanozymes with peroxidase-like activity have been extensively studied for colorimetric biosensing. However, their catalytic activity and specificity still lag far behind those of natural enzymes, which significantly affects the accuracy and sensitivity of colorimetric biosensing. To address this issue, we design PdSn nanozymes with selectively enhanced peroxidase-like activity, which improves the sensitivity and accuracy of a colorimetric immunoassay. The peroxidase-like activity of PdSn nanozymes is significantly higher than that of Pd nanozymes. Theoretical calculations reveal that the p-d orbital hybridization of Pd and Sn not only results in an upward shift of the d-band center to enhance hydrogen peroxide (H2O2) adsorption but also regulates the O-O bonding strength of H2O2 to achieve selective H2O2 activation. Ultimately, the nanozyme-linked immunosorbent assay has been successfully developed to sensitively and accurately detect the prostate-specific antigen (PSA), achieving a low detection limit of 1.696 pg mL-1. This work demonstrates a promising approach for detecting PSA in a clinical diagnosis.
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Técnicas Biossensoriais , Peróxido de Hidrogênio , Masculino , Humanos , Antígeno Prostático Específico , Imunoensaio/métodos , Antioxidantes , Peroxidases , Colorimetria/métodos , Técnicas Biossensoriais/métodosRESUMO
OBJECTIVE: We aimed to explore the heterogeneity of neurons in heart failure with dilated cardiomyopathy (DCM). METHODS: Single-cell RNA sequencing (scRNA-seq) data of patients with DCM and chronic heart failure and healthy samples from GSE183852 dataset were downloaded from NCBI Gene Expression Omnibus, in which neuron data were extracted for investigation. Cell clustering analysis, differential expression analysis, trajectory analysis, and cell communication analysis were performed, and highly expressed genes in neurons from patients were used to construct a protein-protein interaction (PPI) network and validated by GSE120895 dataset. RESULTS: Neurons were divided into six subclusters involved in various biological processes and each subcluster owned its specific cell communication pathways. Neurons were differentiated into two branches along the pseudotime, one of which was differentiated into mature neurons, whereas another tended to be involved in the immune and inflammation response. Genes exhibited branch-specific differential expression patterns. FLNA, ITGA6, ITGA1, and MDK interacted more with other gene-product proteins in the PPI network. The differential expression of FLNA between DCM and control was validated. CONCLUSION: Neurons have significant heterogeneity in heart failure with DCM, and may be involved in the immune and inflammation response to heart failure.
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Cardiomiopatia Dilatada , Insuficiência Cardíaca , Humanos , Cardiomiopatia Dilatada/diagnóstico , Cardiomiopatia Dilatada/genética , Cardiomiopatia Dilatada/metabolismo , Perfilação da Expressão Gênica , Insuficiência Cardíaca/diagnóstico , Insuficiência Cardíaca/genética , Inflamação , Análise de Sequência de RNA , Neurônios/metabolismoRESUMO
The key to increasing the rate of oxygen evolution reaction (OER) lies in accelerated four-electron dynamics, while the key to facilitating the development of supercapacitors lies in the design of electrode materials. This paper synthesized manganese-iron Prussian blue (MnFe-PBA@IF) at room temperature, and hexagonal concave structures w ere prepared using a fast-reducing matrix. Interestingly, MnFe-PBA@IF has an amorphous structure favorable to exposing more active surfaces. According to Gibbs free energy calculations on MnFe-PBA, charge depletion of manganese atoms can greatly enhance the adsorption of electron-rich oxygen-containing groups on the surface. Furthermore, the overpotential in 1 m KOH is 280 mV. Also, it can be used as a supercapacitor with a stable operating voltage range of -0.9-0 V and a specific capacity of 1260 F g-1 . This work provides new insights into the synthesis of OER catalysts for Prussian blue ferromanganese at room temperature. Non-gold-bonded adsorption, highly active metal centers and active surfaces are the underlying reasons for the superior performance of supercapacitors. Therefore, Prussian blue with good energy storage performance and high active surface can be used as multifunctional energy storage and conversion electrodes.
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n-Valeraldehyde is widely used in organic synthesis field as an important intermediate and feedstock, which makes it a significant class of environmental pollutants. In view of the high poisonous and harmful of n-valeraldehyde to human health and ecological environment, it is important to develop green and sustainable technology to reduce the pollution of n-valeraldehyde. In this work, electrocatalytic n-valeraldehyde oxidation using Zn-Co bimetallic oxides was applied to control n-valeraldehyde contamination and highly valuable octane production. To further improve the performance of Zn-Co bimetallic oxides, atomic level Zn vacancies were created across the Zn-Co bimetallic oxides (dx-ZnCo2O4) by post-etching and oxygen vacancy filling methods. Electrochemical experiments results showed that dx-ZnCo2O4 owned a much higher octane yield (1193.4 µmol g-1 h-1) and octane selectivity (octane/butene ≈10). Theoretical calculations demonstrated that the introduction of atomic level Zn vacancies in Zn-Co bimetallic oxide changed the electronic distribution around O, Co and Zn atoms, resulted in an alteration in n-valeraldehyde adsorption sites from Co to Zn, reduced the formation barrier of key intermediate *C4H9 and facilitated the transfer of n-valeraldehyde to octane. This study provides a new idea for the development of high-performance electrocatalysts for controlling n-valeraldehyde pollution.
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Enteral nutrition (EN) is important for critically ill patients. This study investigated the current situation of EN treatment in SHANGHAI intensive care units (ICUs). We hypothesized that improving EN practice in SHANGHAI may benefit the prognosis of ICU patients. Clinical information on EN use was collected using clinic information forms in 2019. The collected data included the patient's general clinical information, EN prescription status, EN tolerance status, and clinical outcomes. The observation time points were days 1, 3, and 7 after starting EN. A total of 491 patients were included. The proportion of EN intolerance (defined as < 20 kcal/kg/day) decreased, with rates of intolerance of 100%, 82.07%, 70.61%, and 52.23% at 1, 3, 7, and 14 days, respectively. Age, mNutric score, and protein intake < 0.5 g/kg/day on day 7 were risk factors for 28-day mortality.The EN tolerance on day 7 and protein intake > 0.5 g/kg/day on day 3 or day 7 might affect the 28-day mortality. Risk factors with EN tolerance on day 7 by logistic regression showed that the AGI grade on day 1 was a major factor against EN tolerance. The proportion of EN tolerance in SHANGHAI ICU patients was low. Achieving tolerance on day 7 after the start of EN is a protective factor for 28-day survival. Improving EN tolerance and protein intake maybe beneficial for ICU patients.
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Cuidados Críticos , Nutrição Enteral , Humanos , Nutrição Enteral/efeitos adversos , China , Unidades de Terapia Intensiva , Estado Nutricional , Estado Terminal/terapiaRESUMO
Sepsis is known to cause damage to the intestinal mucosa, leading to bacterial translocation, and exacerbation of both local and remote organ impairments. In the present study, fecal samples were collected from both septic and healthy individuals. Analysis through 16s rRNA sequencing of the fecal microbiota revealed that sepsis disrupts the balance of the gut microbial community. Recent research has highlighted the association of lipid metabolism with disease. By analyzing the fecal metabolome, four lipid metabolites that showed significant differences between the two groups were identified: PE (O-16:0/0:0), PE (17:0/0:0), PE (0:0/14:0), and PE (12:0/20:5 (5Z, 8Z, 11Z, 14Z, 17Z)). Notably, the serum levels of PE (0:0/14:0) were higher in the healthy group. Subsequent in vitro and in vivo experiments demonstrated the protective effects of this compound against sepsis-induced intestinal barrier damage. Label-free proteomic analysis showed significant differences in the expression levels of the aryl hydrocarbon receptor (AHR), a protein implicated in sepsis pathogenesis, between the LPS-Caco-2 and LPS-Caco-2 + PE (0:0/14:0) groups. Further analysis, with the help of Discovery Studio 3.5 software and co-immunoprecipitation assays, confirmed the direct interaction between AHR and PE (0:0/14:0). In the cecal ligation and puncture (CLP) model, treatment with PE (0:0 /14:0) was found to up-regulate the expression of tight junction proteins through the AHR/Cytochrome P450, family 1, subfamily A, and polypeptide 1 (CYP1A1) pathway. This highlights the potential therapeutic use of PE (0:0/14:0) in addressing sepsis-induced intestinal barrier damage.
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Microbioma Gastrointestinal , Sepse , Humanos , Citocromo P-450 CYP1A1/genética , Citocromo P-450 CYP1A1/metabolismo , Citocromo P-450 CYP1A1/farmacologia , Células CACO-2 , Microbioma Gastrointestinal/fisiologia , Receptores de Hidrocarboneto Arílico/genética , Receptores de Hidrocarboneto Arílico/metabolismo , Receptores de Hidrocarboneto Arílico/uso terapêutico , RNA Ribossômico 16S , Lipopolissacarídeos/farmacologia , Proteômica , Sepse/metabolismo , Mucosa Intestinal/metabolismoRESUMO
Two-dimensional materials are widely used in membrane separation, but the loose distribution and severe expansion between graphene oxide (GO) nanosheets limit its application. Here, we introduce a two-dimensional MOF material into the GO membrane to enhance its water permeance and separation performance. The MOF/GO composite membrane was prepared by vacuum filtration. The MOF and GO nanosheets were tightly stacked through the π-π effect, and the shortened transmission path and enhanced pore structure greatly improved the water permeance of the composite membrane. The MOF/GO membrane exhibited a high water permeance of 56.94 L m-2 h-1 bar-1. The rejection rates of methylene blue and was as methyl orange dyes were as high as 99.79% and 99.11%, respectively. At increased dye concentration, the rejection rate of methylene blue was still maintained greater than 99%. Dye rejection after 18 h of continuous operation remains above 90%. This work provides new ideas for improving membrane separation materials. The combination of two-dimensional heterogeneous materials can result in synergistic advantages for the development of composite membranes with high water permeance and high rejection rate.
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Corantes , Azul de Metileno , Filtração , ÁguaRESUMO
In this study, ZnS capped Cu-In-S (ZCIS) quantum dots doped with Mn ions are synthesized by a thermal injection method, with luminescence covering almost the entire visible area. The large Stokes shift effectively inhibits the self-absorption effect under luminescence, and the quantum yield of ZCIS quantum dots increased from 38% to 50% after ZnS capping and further to 69% after doping with Mn. First, red-, yellow-, and blue-emitting quantum dots were synthesized and then, polychromatic ensembles were obtained by mixing the trichromatic quantum dots in a different ratio. Using the home-built inkjet printer, multilayered and multicolor mixed patterns were obtained for information pattern storage and multilayer pattern recognition and reading.