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A simple, scalable, surfactant-in-polymer templating approach is demonstrated to create controlled long-range secondary substructures in a primary structure. A metal bis(2-ethylhexyl) sulfosuccinate (MAOT) as the surfactant is shown to be capable of serving as a sacrificial template and metal precursor in carbon nanofibers. The low interfacial tension and controllable dimensions of the MAOT are maintained in the solid-phase polymer, even during electrospinning and heat-treatment processes, allowing for the long-range uniform formation of substructures in the nanofibers. The MAOT content is found to be a critical parameter for tailoring the diameter of the nanofibers and their textural properties, such as size and volume of interior pores. The metal counterion species in the MAOT determine the introduction of metallic phases in the nanofiber interior. The incorporation of MAOT with Na as the counterion into the polymer phase leads to the formation of a built-in pore structure in the nanofibers. In contrast, MAOT with Fe as a counterion generates unique iron-in-pore substructures in the nanofibers (FeCNFs). The FeCNFs exhibit outstanding charge storage and water splitting performances. As a result, the MAOT-in-polymer templating approach can be extended to combinations of various metal precursors and thus create desirable functionalities for different target applications.
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The fascinating properties of single-layer graphene isolated by mechanical exfoliation have inspired extensive research efforts toward two-dimensional (2D) materials. Layered compounds serve as precursors for atomically thin 2D materials (briefly, 2D nanomaterials) owing to their strong intraplane chemical bonding but weak interplane van der Waals interactions. There are newly emerging 2D materials beyond graphene, and it is becoming increasingly important to develop cost-effective, scalable methods for producing 2D nanomaterials with controlled microstructures and properties. The variety of developed synthetic techniques can be categorized into two classes: bottom-up and top-down approaches. Of top-down approaches, the exfoliation of bulk 2D materials into single or few layers is the most common. This review highlights chemical and physical exfoliation methods that allow for the production of 2D nanomaterials in large quantities. In addition, remarkable examples of utilizing exfoliated 2D nanomaterials in energy and environmental applications are introduced.
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It is important to fabricate nanostructured architectures comprised of functional components for a wide variety of applications because precise structural control in the nanometer regime can yield unprecedented, fascinating properties. Owing to their well-defined microstructural characteristics, it has been popular to use carbon nanospecies, such as nanotubes and graphene, in fabricating nanocomposites and nanohybrids. Nevertheless, it still remains hard to control and manipulate nanospecies for specific applications, thus preventing their commercialization. Herein, first, we report unique one-dimensional nanoarchitectures with meso-/macropores, consisting of single-walled nanotubes (SWNTs), graphene, and polyacrylonitrile, in which poly(vinyl alcohol) was employed as a dispersing agent and sacrificial porogen. One-dimensional SWNTs and two-dimensional graphene pieces were combined in the confined interior space of electrospun nanofibers, which led to unique microstructural characteristics such as enhanced ordering of SWNTs, graphene pieces, and polymer chains in the nanofiber interior. Next, the SWNT/graphene-in-polymer nanofiber (SGPNF) structures were converted into carbonized products (SGCNFs) with effective porosity and tunable electrochemical properties. Similar to SGPNFs, the microstructural and electrical properties of the SGCNFs depended on the incorporated amount of SWNT and graphene. At higher SWNT content, the mesopore volume proportion and specific discharge capacitance of the SGCNFs increased by max. 63 and 598%, respectively. The SGCNFs showed strong potential as a high-performance electrode material for electrochemical capacitors (max. capacitance: nonactivated â¼390 F g-1 and activated â¼750 F g-1). Flexible, all solid-state capacitor cells based on SGCNFs were also successfully demonstrated as a model application. The SGCNFs can be further functionalized by various methods, which will impart attractive properties for extended applications.
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BACKGROUND: There are currently two markers used to monitor treatment response to anti-retroviral therapy (ART) in HIV-infected children: CD4 T-cell count and HIV viral load; but analysis of these could be challenging in resource-poor countries. The aim of this study was therefore to determine whether change in growth parameters such as weight-for-age Z score (WAZ), height-for-age Z score (HAZ) and body mass index-for-age Z score (BMIZ) is associated with treatment response in HIV-infected children. METHODS: This was a nested case-control study, in which the data were collected at enrolment and then periodically every 6 months for a total 36 month follow up of 107 HIV-infected children enrolled and treated at National Hospital of Pediatrics, Vietnam. RESULTS: At treatment initiation, WAZ, HAZ and BMIZ were not significantly higher in the treatment success (TS) group compared with the treatment failure (TF) group. After ART initiation, WAZ and HAZ increased, and this was significant in the TS group (from -1.5 to -0.54, P < 0.01 and from -2.06 to -0.84, P < 0.01, respectively). Low HAZ was significantly associated with TF (HR, 0.71; 95% CI: 0.54-0.92). CONCLUSION: Height-for-age Z score was the most sensitive growth parameter in prediction of the treatment response. In order to use growth parameters, particularly HAZ as a prognosis marker for TF in clinical practice, further research should be conducted to evaluate the role of growth parameters and their effects on treatment response.
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Antirretrovirais/uso terapêutico , Desenvolvimento Infantil/efeitos dos fármacos , Infecções por HIV/tratamento farmacológico , Antropometria , Estudos de Casos e Controles , Criança , Pré-Escolar , Feminino , Seguimentos , Infecções por HIV/fisiopatologia , Humanos , Lactente , Masculino , Resultado do Tratamento , VietnãRESUMO
Intriguingly, coordination polymers containing TCNQ(2) and TCNQF4(2) (TCNQ = 7,7,8,8-tetracyanoquinodimethane, TCNQF4 = 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, both designated as TCNQ(F4)(2)) may be generated from reaction of metal ions with TCNQ(F4)â¢. An explanation is now provided in terms of a solvent-dependent dynamic disproportionation reaction. A systematic study of reactions associated with TCNQ(F4) and electrochemically generated TCNQ(F4)MeCN⢠and TCNQ(F4)MeCN(2) revealed that disproportionation of TCNQ(F4)MeCN⢠radical anions in acetonitrile containing a low concentration of water is facilitated by the presence of ZnMeCN(2+). Thus, while the disproportionation reaction 2TCNQ(F4)MeCN⢠TCNQ(F4)MeCN + TCNQ(F4)MeCN(2) is thermodynamically very unfavorable in this medium (Keq ≈ 9 × 10(10); TCNQF4), the preferential precipitation of ZnTCNQ(F4)(s) drives the reaction: ZnMeCN(2+) + 2 TCNQ(F4)MeCN⢠ZnTCNQ(F4)(s) + TCNQ(F4)MeCN. The concomitant formation of soluble TCNQ(F4)MeCN and insoluble ZnTCNQ(F4)(s) and the loss of TCNQ(F4)MeCN⢠were verified by UVvisible and infrared spectroscopy and steady-state voltammetry. Importantly, the reverse reaction of comproportionation rather than disproportionation becomes the favored process in the presence of ≥3% (v/v) water, due to the increased solubility of solid ZnTCNQ(F4)(s). Thus, in this "wet" environment, ZnMeCN(2+) and TCNQ(F4)MeCN⢠are produced from a mixture of ZnTCNQ(F4)(s) and TCNQ(F4)MeCN and with the addition of water provides a medium for synthesis of [Zn(TCNQ(F4))2(H2O)2]. An important conclusion from this work is that the redox level of TCNQ(F4)-based materials, synthesized from a mixture of metal cations and TCNQ(F4)â¢, is controlled by a solvent-dependent disproportionation/comproportionation reaction that may be tuned to favor formation of solids containing the monoanion radical, the dianion, or even a mixture of both.
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The past decade has witnessed a rapid rise in the performance of optoelectronic devices based on lead-halide perovskites (LHPs). The large mobility-lifetime products and defect tolerance of these materials, essential for optoelectronics, also make them well-suited for radiation detectors, especially given the heavy elements present, which is essential for strong X-ray and γ-ray attenuation. Over the past decade, LHP thick films, wafers, and single crystals have given rise to direct radiation detectors that have outperformed incumbent technologies in terms of sensitivity (reported values up to 3.5 × 106 µC Gyair -1 cm-2 ), limit of detection (directly measured values down to 1.5 nGyair s-1 ), along with competitive energy and imaging resolution at room temperature. At the same time, lead-free perovskite-inspired materials (e.g., methylammonium bismuth iodide), which have underperformed in solar cells, have recently matched and, in some areas (e.g., in polarization stability), surpassed the performance of LHP detectors. These advances open up opportunities to achieve devices for safer medical imaging, as well as more effective non-invasive analysis for security, nuclear safety, or product inspection applications. Herein, the principles behind the rapid rises in performance of LHP and perovskite-inspired material detectors, and how their properties and performance link with critical applications in non-invasive diagnostics are discussed. The key strategies to engineer the performance of these materials, and the important challenges to overcome to commercialize these new technologies are also discussed.
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In this study, we investigated the possibility of a photocatalytic system that uses graphene-quantum-dot (GQD)-deposited graphitic carbon nitride (g-C3N4) to treat tetracycline (TC) and other organic compounds generated from an in-situ-recirculatory-aquaculture-system (RAS)-like shrimp farming pond. GQDs were successfully deposited on the exfoliated g-C3N4 base through a hydrothermal treatment. The results showed that the incorporation of GQDs into the g-C3N4 enhanced its porosity without aggregating its mesoporous structure. The GQDs-deposited g-C3N4 photocatalysts revealed sheet-like structures with nanopores on their surface that facilitate photocatalysis. More than 90% of the TC was removed by the photocatalysts under UV-LED irradiation. Low loadings of GQDs over g-C3N4 resulted in a faster and more effective photocatalysis of TC, mainly driven by.O2- radicals. The photocatalysts were also applicable in the degradation of organic compounds with 27% of the total organic compounds (TOC) being removed from the wastewater of a RAS-like shrimp farming pond.
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One of the various sorts of damage to asphalt concrete is cracking. Repeated loads, the deterioration or aging of material combinations, or structural factors can contribute to the development of cracks. Asphalt concrete's crack resistance is represented by the CT index. 107 CT Index data samples from the University of Transport Technology's lab are measured. These data samples are used to establish a database from which a Machine Learning (ML) model for predicting the CT Index of asphalt concrete can be built. For creating the highest performing machine learning model, three well-known machine learning methods are introduced: Random Forest (RF), K-Nearest Neighbors (KNN), and Multivariable Adaptive Regression Spines (MARS). Monte Carlo simulation is used to verify the accuracy of the ML model, which includes the Root Mean Square Error (RMSE), Mean Absolute Error (MAE), Mean Absolute Percentage Error (MAPE), and coefficient of determination (R2). The RF model is the most effective ML model, according to analysis and evaluation of performance indicators. By SHAPley Additive exPlanations based on RF model, the input Aggregate content passing 4.75 mm sieve (AP4.75) has a significant effect on the variation of CT Index value. In following, the descending order is Reclaimed Asphalt Pavement content (RAP) > Bitumen content (BC) > Flash point (FP) > Softening point > Rejuvenator content (RC) > Aggregate content passing 0.075mm sieve (AP0.075) > Penetration at 25°C (P). The results study contributes to selecting a suitable AI approach to quickly and accurately determine the CT Index of asphalt concrete mixtures.
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Aprendizado de Máquina , Movimento Celular , Análise por ConglomeradosRESUMO
The crystallization of nanocrystal building blocks into artificial superlattices has emerged as an efficient approach for tailoring the nanoscale properties and functionalities of novel devices. To date, ordered arrays of colloidal metal halide nanocrystals have mainly been achieved by using post-synthetic strategies. Here, a rapid and direct liquid-phase synthesis is presented to achieve a highly robust crystallization of luminescent metal halide nanocrystals into perfect face-centered-cubic (FCC) superlattices on the micrometer scale. The continuous growth of individual nanocrystals is observed within the superlattice, followed by the disassembly of the superlattices into individually dispersed nanocrystals owing to the highly repulsive interparticle interactions induced by large nanocrystals. Transmission electron microscopy characterization reveals that owing to an increase in solvent entropy, the structure of the superlattices transforms from FCC to hexagonal close-packed (HCP) and the nanocrystals disassemble. The FCC superlattice exhibits a single and slightly redshifted emission, due to the reabsorption-free property of the building block units. Compared to individual nanocrystals, the superlattices have three times higher quantum yield with improved environmental stability, making them ideal for use as ultrabright blue-light emitters. This study is expected to facilitate the creation of metamaterials with ordered nanocrystal structures and their practical applications.
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Polarimetric imaging systems combining machine learning is emerging as a promising tool for the support of diagnosis and intervention decision-making processes in cancer detection/staging. A present study proposes a novel method based on Mueller matrix imaging combining optical parameters and machine learning models for classifying the progression of skin cancer based on the identification of three different types of mice skin tissues: healthy, papilloma, and squamous cell carcinoma. Three different machine learning algorithms (K-Nearest Neighbors, Decision Tree, and Support Vector Machine (SVM)) are used to construct a classification model using a dataset consisting of Mueller matrix images and optical properties extracted from the tissue samples. The experimental results show that the SVM model is robust to discriminate among three classes in the training stage and achieves an accuracy of 94 % on the testing dataset. Overall, it is provided that polarimetric imaging systems and machine learning algorithms can dynamically combine for the reliable diagnosis of skin cancer.
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The chemistry and electrochemistry of TCNQ (7,7,8,8-tetracyanoquinodimethane), TCNQ(â¢-), TCNQ(2-), and H(2)TCNQ in acetonitrile (0.1 M Bu(4)NPF(6)) solution containing trifluoroacetic acid (TFA) has been studied by transient and steady-state voltammetric methods with the interrelationship between the redox and the acid-base chemistry being supported by simulations of the cyclic voltammograms. In the absence of acid, TCNQ and its anions undergo two electrochemically and chemically reversible one-electron processes. However, in the presence of TFA, the voltammetry is considerably more complex. The TCNQ(2-) dianion is protonated to form HTCNQ(-), which is oxidized to HTCNQ(â¢), and H(2)TCNQ which is electroinactive over the potential range of -1.0 to +1.0 V versus Ag/Ag(+). The monoreduced TCNQ(â¢-) radical anion is weakly protonated to give HTCNQ(â¢), which disproportionates to TCNQ and H(2)TCNQ. In acetonitrile, H(2)TCNQ deprotonates slowly, whereas in N,N-dimethylformamide or tetrahydrofuran, rapid deprotonation occurs to yield HTCNQ(-) as the major species. H(2)TCNQ is fully deprotonated to the TCNQ(2-) dianion in the presence of an excess concentration of the weak base, CH(3)COOLi. Differences in the redox and acid-base chemistry relative to the fluorinated derivative TCNQF(4) are discussed in terms of structural and electronic factors.
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Careful control of the reaction stoichiometry and conditions enables the synthesis of both LiTCNQF(4) and Li(2)TCNQF(4) to be achieved. Reaction of LiI with TCNQF(4), in a 4:1 molar ratio, in boiling acetonitrile yields Li(2)TCNQF(4). However, deviation from this ratio or the reaction temperature gives either LiTCNQF(4) or a mixture of Li(2)TCNQF(4) and LiTCNQF(4). This is the first report of the large-scale chemical synthesis of Li(2)TCNQF(4). Attempts to prepare a single crystal of Li(2)TCNQF(4) have been unsuccessful, although air-stable (Pr(4)N)(2)TCNQF(4) was obtained by mixing Pr(4)NBr with Li(2)TCNQF(4) in aqueous solution. Pr(4)NTCNQF(4) was also obtained by reaction of LiTCNQF(4) with Pr(4)NBr in water. Li(2)TCNQF(4), (Pr(4)N)(2)TCNQF(4), and Pr(4)NTCNQF(4) have been characterized by UV-vis, FT-IR, Raman, and NMR spectroscopy, high resolution electrospray ionization mass spectrometry, and electrochemistry. The structures of single crystals of (Pr(4)N)(2)TCNQF(4) and Pr(4)NTCNQF(4) have been determined by X-ray crystallography. These TCNQF(4)(2-) salts will provide useful precursors for the synthesis of derivatives of the dianions.
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Compostos de Lítio/síntese química , Compostos de Amônio Quaternário/síntese química , Compostos de Tecnécio/síntese química , Cristalografia por Raios X , Eletroquímica , Compostos de Lítio/química , Espectroscopia de Ressonância Magnética , Estrutura Molecular , Compostos de Amônio Quaternário/química , Compostos de Tecnécio/químicaRESUMO
Flexible sensing devices have attracted significant attention for various applications, such as medical devices, environmental monitoring, and healthcare. Numerous materials have been used to fabricate flexible sensing devices and improve their sensing performance in terms of their electrical and mechanical properties. Among the studied materials, conductive polymers are promising candidates for next-generation flexible, stretchable, and wearable electronic devices because of their outstanding characteristics, such as flexibility, light weight, and non-toxicity. Understanding the interesting properties of conductive polymers and the solution-based deposition processes and patterning technologies used for conductive polymer device fabrication is necessary to develop appropriate and highly effective flexible sensors. The present review provides scientific evidence for promising strategies for fabricating conductive polymer-based flexible sensors. Specifically, the outstanding nature of the structures, conductivity, and synthesis methods of some of the main conductive polymers are discussed. Furthermore, conventional and innovative technologies for preparing conductive polymer thin films in flexible sensors are identified and evaluated, as are the potential applications of these sensors in environmental and human health monitoring.
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Significance: The combination of polarized imaging with artificial intelligence (AI) technology has provided a powerful tool for performing an objective and precise diagnosis in medicine. Aim: An approach is proposed for the detection of hepatitis B (HB) virus using a combined Mueller matrix imaging technique and deep learning method. Approach: In the proposed approach, Mueller matrix imaging polarimetry is applied to obtain 4 × 4 Mueller matrix images of 138 HBsAg-containing (positive) serum samples and 136 HBsAg-free (negative) serum samples. The kernel estimation density results show that, of the 16 Mueller matrix elements, elements M 22 and M 33 provide the best discriminatory power between the positive and negative samples. Results: As a result, M 22 and M 33 are taken as the inputs to five different deep learning models: Xception, VGG16, VGG19, ResNet 50, and ResNet150. It is shown that the optimal classification accuracy (94.5%) is obtained using the VGG19 model with element M 22 as the input. Conclusions: Overall, the results confirm that the proposed hybrid Mueller matrix imaging and AI framework provides a simple and effective approach for HB virus detection.
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Inteligência Artificial , Hepatite B , Humanos , Hepatite B/diagnóstico por imagem , Diagnóstico por ImagemRESUMO
The electrochemistry of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (TCNQF(4)), [TCNQF(4)](â¢-), and [TCNQF(4)](2-) have been studied in acetonitrile (0.1 M [Bu(4)N][ClO(4)]). Transient and steady-state voltammetric techniques have been utilized to monitor the generation of [TCNQF(4)](â¢-) and [TCNQF(4)](2-) anions as well as their reactions with trifluoroacetic acid (TFA). In the absence of TFA, the reduction of TCNQF(4) occurs via two, diffusion controlled, chemically and electrochemically reversible, one-electron processes where the reversible formal potentials are 0.31 and -0.22 V vs Ag/Ag(+). Unlike the TCNQ analogues, both [TCNQF(4)](â¢-) and [TCNQF(4)](2-) are persistent when generated via bulk electrolysis even under aerobic conditions. Voltammetric and UV-vis data revealed that although the parent TCNQF(4) does not react with TFA, the electrochemically generated radical anion and dianion undergo facile protonation to yield [HTCNQF(4)](â¢), [HTCNQF(4)](-) and H(2)TCNQF(4) respectively. The voltammetry can be simulated to give a complete thermodynamic and kinetic description of the complex, coupled redox and acid-base chemistry. The data indicate dramatically different equilibrium and rate constants for the protonation of [TCNQF(4)](â¢-) (K(eq) = 3.9 × 10(-6), k(f) = 1.0 × 10(-3) M(-1) s(-1)) and [TCNQF(4)](2-) (K(eq) = 3.0 × 10(3), k(f) = 1.0 × 10(10) M(-1) s(-1)) in the presence of TFA.
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SIGNIFICANCE: The Mueller matrix decomposition method is widely used for the analysis of biological samples. However, its presumed sequential appearance of the basic optical effects (e.g., dichroism, retardance, and depolarization) limits its accuracy and application. AIM: An approach is proposed for detecting and classifying human melanoma and non-melanoma skin cancer lesions based on the characteristics of the Mueller matrix elements and a random forest (RF) algorithm. APPROACH: In the proposal technique, 669 data points corresponding to the 16 elements of the Mueller matrices obtained from 32 tissue samples with squamous cell carcinoma (SCC), basal cell carcinoma (BCC), melanoma, and normal features are input into an RF classifier as predictors. RESULTS: The results show that the proposed model yields an average precision of 93%. Furthermore, the classification results show that for biological tissues, the circular polarization properties (i.e., elements m44, m34, m24, and m14 of the Mueller matrix) dominate the linear polarization properties (i.e., elements m13, m31, m22, and m41 of the Mueller matrix) in determining the classification outcome of the trained classifier. CONCLUSIONS: Overall, our study provides a simple, accurate, and cost-effective solution for developing a technique for classification and diagnosis of human skin cancer.
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Carcinoma , Neoplasias Cutâneas , Algoritmos , Humanos , Fenômenos Ópticos , PeleRESUMO
CsPbBr3 perovskite nanocrystals with two different dimensionalities were synthesized at different temperatures and then integrated as optoelectronic transducers into transistor-type photoconversion devices. Postsynthesis transformation was observed for two-dimensional (2D) nanoplatelets, while the transformation was rarely found in 3D nanocubes. At ambient temperature and pressure, neighboring nanoplatelets made facet-to-facet contact and then fused into larger 2D nanoplatelets (2-5 times) without defects. The coalescence of 2D nanoplatelets at the ambient condition lowered the density of defects at the surface of the nanocrystals and thus could facilitate effective and stable photoconversion behavior in the nanocrystal film integrated into the device. Consequently, the ambient-condition aging of 2D nanoplatelets on device substrate led to 3 times higher retention in photoconversion performance. Importantly, these results provide a new concept of how perovskite nanocrystals can be integrated into a device for enhanced stability in device performance.
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The evolution of influenza viruses is fundamentally shaped by within-host processes. However, the within-host evolutionary dynamics of influenza viruses remain incompletely understood, in part because most studies have focused on infections in healthy adults based on single timepoint data. Here, we analyzed the within-host evolution of 82 longitudinally sampled individuals, mostly young children, infected with A/H1N1pdm09 or A/H3N2 viruses between 2007 and 2009. For A/H1N1pdm09 infections during the 2009 pandemic, nonsynonymous minority variants were more prevalent than synonymous ones. For A/H3N2 viruses in young children, early infection was dominated by purifying selection. As these infections progressed, nonsynonymous variants typically increased in frequency even when within-host virus titers decreased. Unlike the short-lived infections of adults where de novo within-host variants are rare, longer infections in young children allow for the maintenance of virus diversity via mutation-selection balance creating potentially important opportunities for within-host virus evolution.
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Evolução Molecular , Vírus da Influenza A/genética , Influenza Humana/epidemiologia , Pandemias , Adolescente , Criança , Pré-Escolar , Humanos , Influenza Humana/virologia , Estações do Ano , Vietnã/epidemiologia , Adulto JovemRESUMO
Correction for 'Pine cone mold: a toolbox for fabricating unique metal/carbon nanohybrid electrocatalysts' by Hyunwoo Han et al., Nanoscale, 2019, DOI: 10.1039/c9nr06794a.
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The functionalization of nanocarbon materials such as graphene has attracted considerable attention over the past decades. In this work, we designed and synthesized a unique N-heterocyclic carbene compound with a pyrene tail group (NHCp) to investigate how carbene species can be used for the functionalization of graphene. Although the carbene moiety of NHCp has the ability to covalently bond to graphene, the pyrene tail can noncovalently interact with graphene and allows monitoring its surrounding microenvironment. The major characteristics of the resulting nanohybrids were highly dependent on the type of graphene and the NHCp-to-graphene weight ratio. Importantly, despite the covalent functionalization of graphene, an anomalous decrease in the intensity of the Raman D peak and improved conductivity were observed for the nanohybrids. It was found that the covalent bond of NHCp to the graphene edge may allow the hybridization of their orbitals, which affects electronic energy levels and alters the double resonance process that originates the D peak at the edge defect. Importantly, the NHCp compound can act as a π acceptor (not just as a σ donor) via the NHCp-graphene covalent bridge. This is the first report showing that the concept of π-backdonation can be realized in two-dimensional materials, such as graphene, and rationally designed carbene molecules can functionalize graphene without losing their beneficial sp2 hybridization characteristics.