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Explanation for the modification of rates and mechanism of reactions carried out in optical cavities still eludes us. Several studies indicate that the cavity-mediated changes in the nature of vibrational energy flow within a molecule may play a significant role. Here, we study a model polaritonic system, proposed and analyzed earlier by Fischer et al., J. Chem. Phys. 156, 154305 (2022), comprising a one-dimensional isomerization mode coupled to a single photon mode in a lossless cavity. We show that the isomerization probability in the presence of virtual photons, for specific cavity-system coupling strengths and cavity frequencies, can exhibit suppression or enhancement for different choices of the initial reactant vibropolariton wavepacket. We observe a qualitative agreement between the classical and quantum average isomerization probabilities in the virtual photon case. A significant part of the effects due to coupling to the cavity can be rationalized in terms of a "chaos-order-chaos" transition of the classical phase space and the phase space localization nature of the polariton states that dominantly participate in the quantum isomerization dynamics. On the other hand, for initial states with zero photons (i.e., a "dark cavity"), the isomerization probability is suppressed when the cavity frequency is tuned near to the fundamental frequency of the reactive mode. The classical-quantum correspondence in the zero photon case is unsatisfactory. In this simple model, we find that the suppression or enhancement of isomerization arises due to the interplay between cavity-system energy flow dynamics and quantum tunneling.
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We study the dissociation dynamics of a diatomic molecule, modeled as a Morse oscillator, coupled to an optical cavity. A marked suppression of the dissociation probability, both classical and quantum, is observed for cavity frequencies significantly below the fundamental transition frequency of the molecule. We show that the suppression in the probability is due to the nonlinearity of the dipole function. The effect can be rationalized entirely in terms of the structures in the classical phase space of the model system.
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We report on metal-non-metal doped carbon dots with very high photoluminescent properties in solution. Magnesium doping to tamarind extract associated with nitrogen-doping is for the first time reported here which also produce very high quantum yield. Our aim is to develop such dual doped carbon dots which can also serve living cell imaging with easy permeation towards cells and show non-cytotoxic attributes. More importantly, the chemical signatures of the carbon dots unveiled in this work can support their easy solubilization into water; even in sub-ambient temperature. The cytotoxicity assay proves the almost negligible cytotoxic effect against human cell lines. Moreover, the use of carbon dots in UV-active marker and polymer composites are also performed which gave clear distinguishable features of fluorescent nanoparticles. Hitherto, the carbon dots can be commercially prepared without adopting any rigorous methods and also can be used as non-photo-bleachable biomarkers of living cells.
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Materiales Biocompatibles/química , Carbono/química , Color , Sustancias Luminiscentes/química , Polímeros/química , Puntos Cuánticos/química , Línea Celular , Fluorescencia , Humanos , Rayos UltravioletaRESUMEN
Fluorescent carbon dots, zero-dimensional nanomaterials with surface ligands, have been studied extensively over the past few years in biolabelling or fluorescence-based live cell assays. In the past, synthetic organic dyes have been used as cell tracking materials, but they have severe limitations; fluorescent carbon dots may pave the way to biolabelling and cell imaging. In this work, green fluorescent carbon dots have been synthesized from a green source, gram, without any sort of covalent or ionic modifications. These gram-derived carbon dots are unique with respect to synthetic commercial cell-tracking dyes as they are non-toxic, cell internalization occurs quickly, and they have excellent bioconjugation with bacterial cells. Our aim is to establish these carbon dots in a biolabelling assay with its other physicochemical features like the tunable luminescence property, high degree of water solubility and low toxicity, towards various environments (wide range of pH, high ionic strength). Our study introduces a new perspective on the commercialization of carbon dots as a potential alternative to synthetic organic dyes for fluorescence-based cell-labelling assays.
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Carbono/química , Cicer/química , Escherichia coli/ultraestructura , Colorantes Fluorescentes/química , Imagen Molecular/métodos , Puntos Cuánticos/química , Escherichia coli/efectos de los fármacos , Escherichia coli/metabolismo , Colorantes Fluorescentes/aislamiento & purificación , Tecnología Química Verde , Concentración de Iones de Hidrógeno , Mediciones Luminiscentes , Viabilidad Microbiana/efectos de los fármacos , Concentración Osmolar , Extractos Vegetales/química , Solubilidad , ResiduosRESUMEN
The fabrication of scalable and affordable conductive Ketjen carbon black (K-CB)-elastomer composites for adjustable electromagnetic interference (EMI) shielding remains a difficult challenge. Herein, chlorinated polyethylene (CPE)-K-CB composites have been developed by single step solution mixing to achieve high EMI shielding performance associated with absorption dominance potency by conductive dissipation as well as the reflection of electromagnetic waves. The dispersion of K-CB inside the CPE matrix has been corroborated by electron micrographs and atomic force microscopy (AFM). The K-CB filler and CPE polymer interaction has been investigated through the bound rubber content (Bdr) and the dynamic mechanical properties. The relatively low loading of K-CB with respect to other conventional carbon fillers contributes to a promising low percolation threshold (9.6 wt% K-CB) and a reasonably high EMI shielding effectiveness (EMI SE) value of 38.4 dB (at 30 wt% loading) in the X-band region (8.2 to 12.4 GHz). Classical percolation theory reveals that the electrical conduction behavior through the composite system is quasi-two dimensional in nature. Our belief lies in the promotion of scalable production of flexible and cost-effective K-CB-CPE composites of superior EMI SE to avoid electromagnetic radiation pollution.
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The impact of electron beam radiation on the blend of linear low-density polyethylene (LLDPE) and polydimethylsiloxane (PDMS) rubber at different doses from 50 to 300 kGy has been investigated. The irradiated sheets were examined for their morphology, gel content, thermal stability, melt behavior, and electrical and dielectric properties. The radiation treatment has reduced both the melting point and crystallinity of base polymers and their blends because of chain scission. As observed, 100 kGy doses of irradiated blend and 3 wt % of loaded nanosilica composite showed comparatively good thermal stability. The phase morphology of the LLDPE: PDMS rubber blend showed a honeycomb-like design before irradiation because of two-stage morphology, which prominently changed into a solitary stage after electron beam irradiation. This is because of intermolecular cross-link arrangement inside the singular parts, just like cross-linking development at the interface. From the AQFESEM study, it is observed that the stacking of nanosilica particles within the blend matrix is greatly reduced after electron beam irradiation. The addition of nanosilica within the blend increased the electrical conductivity and dielectric permittivity. The dielectric breakdown strength has been observed to be the highest for 3 wt % loaded nanocomposite and its irradiated sample. The result indicates that the nanocomposite can be utilized for high-voltage cable applications in indoor and outdoor fields.
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Anticancer drugs are often associated with limitations such as poor stability in aqueous solutions, limited cell membrane permeability, nonspecific targeting, and irregular drug release when taken orally. One possible solution to these problems is the use of nanocarriers of drug molecules, particularly those with targeting ability, stimuli-responsive properties, and high drug loading capacity. These nanocarriers can improve drug stability, increase cellular uptake, allow specific targeting of cancer cells, and provide controlled drug release. While improving the therapeutic efficacy of cancer drugs, contemporary researchers also aim to reduce their associated side effects, such that cancer patients are offered with a more effective and targeted treatment strategy. Herein, a set of nine porous covalent organic frameworks (COFs) were tested as drug delivery nanocarriers. Among these, paclitaxel loaded in COF-3 was most effective against the proliferation of ovarian cancer cells. This study highlights the emerging potential of COFs in the field of therapeutic drug delivery. Due to their biocompatibility, these porous COFs provide a viable substrate for controlled drug release, making them attractive candidates for improving drug delivery systems. This work also demonstrates the potential of COFs as efficient drug delivery agents, thereby opening up new opportunities in the field of sarcoma therapy.
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Antineoplásicos , Portadores de Fármacos , Estructuras Metalorgánicas , Neoplasias Ováricas , Paclitaxel , Humanos , Neoplasias Ováricas/tratamiento farmacológico , Neoplasias Ováricas/metabolismo , Portadores de Fármacos/química , Femenino , Antineoplásicos/uso terapéutico , Antineoplásicos/química , Antineoplásicos/farmacología , Paclitaxel/uso terapéutico , Paclitaxel/química , Paclitaxel/farmacología , Estructuras Metalorgánicas/química , Estructuras Metalorgánicas/uso terapéutico , Estructuras Metalorgánicas/farmacología , Línea Celular Tumoral , Porosidad , Liberación de FármacosRESUMEN
Herein, we report an efficient synthetic strategy for an Fe(ii)-catalyzed site-selective ring opening of bicyclo[n.1.0]alkanols and their concomitant 1,6-conjugate addition to p-quinone methides. Access to tertiary carbon centers with appendaged carbocycles of distinct sizes and functional groups are achieved, under a substrate-controlled bond scission of the fused cyclopropanols. Synthetic derivatizations further enhance the utility of the protocol.
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The hydrogen-bonded network of water can be affected both structurally and dynamically by the presence of ions. In the present study, we have considered three aqueous solutions of metal nitrates to investigate the effects of divalent cations (Mg2+ and Ca2+), compared to that of monovalent Na+ ions, on hydrogen-bond fluctuations and vibrational spectral diffusion through calculations of linear and two-dimensional infrared spectra of these solutions at room temperature. We have employed the methods of molecular dynamics simulations using effective polarizable models of ions combined with quantum mechanical calculations of transition variables and statistical mechanical calculations of spectral response functions of vibrational spectroscopy. Divalent cations are found to have much stronger and longer-ranged effects on the structure and dynamics of the hydrogen-bonded network than that induced by the monovalent sodium ions. The blue shifts in the calculated linear spectra are found to follow the Hofmeister trend for the cations. The 2D-IR spectral lineshape and intensity corresponding to three-pulse echo peak shift (3PEPS) experiments are calculated. The timescales of these nonlinear spectral responses and also frequency-time correlations show significant slowing down of spectral diffusion for solutions containing divalent Mg2+ and Ca2+ ions compared to the corresponding dynamics of the solution containing Na+ ions. Unlike NaNO3 solution, the relaxation of frequency and dipole orientational fluctuations of anion-bound water in Mg(NO3)2 and Ca(NO3)2 solutions are found to be somewhat slower than bulk water, which can be attributed to the presence of divalent cations whose effects go beyond their first solvation shells. This is also seen in the dynamics of bulk water in these solutions which is found to be notably slower for the solutions containing divalent cations than that in the NaNO3 solution. Unlike Mg2+ and Ca2+ ions, no specific cationic effect is observed for the Na+ ions.
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Macroporous hydrogel monoliths having tailor-made features, conductivity, superstretchability, excellent biocompatibility, and biodegradability, have become the most nurtured field of interest in soft biomaterials. Green method assisted reduced graphene oxide has been inserted by in situ free radical gelation into semi-IPN hydrogel matrix to fabricate conducting hydrogel. Mechanical toughness has been implemented for the graphene-polymer physisorption interactions with graphene basal planes. Moreover, the as-prepared 3D scaffold type monolith hydrogel has been rheologically superior regarding their high elastic modulus and delayed gel rupturing. κ-Carragenaan, one of the components of the hydrogel, has biodegradable nature. The most significant outcome is their low electrical percolation threshold and reversibly ductile nature. Reversible ductility provides them with rubber-like consistency in flow conditions. Surprising, the hydrogels showed dual stimuli-responsiveness, that is, environmental pH and external electrical stimulation. Electro-stimulation has been adopted here for the first time in semi-IPN systems, which could be an ideal alternative for iontopheretic devices and pulsatile drug release through skin. Regarding this, the hydrogel also has been passed to biocompatibility assay; they are noncytotoxic and show cell proliferation without negligible cell death in live-dead assay. The porosity of the nanocomposite scaffold-like gels was also analyzed by microcomputed tomography (µ-CT), which exhibited their connectivity in cell/voids inside the matrix. Thus, the experimentations are on the support of biocompatible soft material for dual-responsive tunable drug delivery.
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Portadores de Fármacos/química , Grafito/química , Hidrogeles/química , Materiales Biocompatibles/química , Materiales Biocompatibles/farmacología , Carragenina/química , Línea Celular Tumoral , Proliferación Celular/efectos de los fármacos , Liberación de Fármacos , Conductividad Eléctrica , Humanos , Concentración de Iones de Hidrógeno , Muramidasa/química , Muramidasa/metabolismo , Nanocompuestos/química , Nanocompuestos/toxicidad , Porosidad , Reología , Agua/químicaRESUMEN
Nanoparticles embedded semi-interpenetrating (semi-IPNs) polymeric hydrogels with enhanced mechanical toughness and biocompatibility could have splendid biomedical acceptance. Here we propose poly(methacrylic acid) grafted polysaccharide based semi-IPNs filled with nanoclay via in situ Michael type reaction associated with covalent crosslinking with N,N-methylenebisacrylamide (MBA). The effect of nanoclay in the semi-IPN hydrogel has been investigated which showed significant improvement of mechanical robustness. Meanwhile, the hydrogels showed reversible ductility up to 70% in response to cyclic loading-unloading cycle which is an obvious phenomenon of rubber-like elasticity. The synthesized semi-IPN hydrogel show biodegradability and non-cytotoxic nature against human cells. The live-dead assay showed that the prepared hydrogel is a viable platform for cell growth without causing severe cell death. The in vitro drug release study in psychological pH (pHâ¯=â¯7.4) reveals that the controlled drug release phenomena can be tuned by simulating the environment pH. Such features in a single hydrogel assembly can propose this as high performance; biodegradable and non-cytotoxic 3D scaffold based promising biomaterial for tissue engineering.
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Materiales Biocompatibles/química , Portadores de Fármacos/química , Hidrogeles/química , Preparaciones Farmacéuticas/química , Ácidos Polimetacrílicos/química , Polisacáridos/química , Acrilamidas/química , Materiales Biocompatibles/farmacología , Línea Celular , Supervivencia Celular/efectos de los fármacos , Liberación de Fármacos , Elastómeros , Humanos , Hidrogeles/farmacología , Concentración de Iones de Hidrógeno , Preparaciones Farmacéuticas/metabolismo , Polímeros/química , Reología , Temperatura , Resistencia a la Tracción , Teofilina/química , Teofilina/metabolismoRESUMEN
Soft biomaterials derived from polysaccharides are generally suffers from lack of mechanical robustness and instability. The naturally occurring highly abundance low cost polysaccharide has immense aspect as biomaterial after functionalization which can be designed as stretchable and rubber-like elastic with reversible ductility. A highly swellable, stretchable, low creep, non-cytotoxic nanocomposite hydrogel has been fabricated by simple one-pot Michael type covalent grafting of acrylic acid based copolymer onto psyllium biomacromolecular chian by free radical gelation technique. The fabricated hydrogel was rheologically tested which implies its viscoelastic and thixotropic like features. The porous morphology of the hydrogel was confirmed by scanning electron micrograph. The cryo-transmission electron micrograph shows the random dispersion of the nanoclay (cloisite 10A) tactoids in exfoliated as well intercalated forms. These random distributions of clay nanosheets also enhance the mechanical toughness and reversible ductility of the hydrogels which was also supported by the mechanical and loading-unloading cycle measurement. Nonetheless, the nanocomposite hydrogel was non-cytotoxic against human cell-line (human osteosarcoma) and shows good cell attachment of live cells in a 5-day 'live-dead' assay with almost negligible quantity of cell death. These attributes can promote this material as a soft biomaterial for controlled release device with mechanical robustness and rubber-like elasticity.
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Liberación de Fármacos , Hidrogel de Polietilenoglicol-Dimetacrilato/química , Nanocompuestos/química , Psyllium/química , Resinas Acrílicas/química , Silicatos de Aluminio/química , Arcilla , Portadores de Fármacos , Humanos , Hidrogel de Polietilenoglicol-Dimetacrilato/uso terapéutico , Polímeros/química , Polímeros/uso terapéutico , Porosidad , Reología , Sodio/químicaRESUMEN
Nanohybrid hydrogels based on pristine graphene with enhanced toughness and dual responsive drug delivery feature is opening a new era for smart materials. Here pristine graphene hydrogels are synthesized by in situ free radical polymerization where graphene platelets are the nanobuiliding blocks to withstand external stress and shows reversible ductility. Such uniqueness is a mere reflection of rubber-like elasticity on the hydrogels. These nanobuilding blocks serve also the extensive physisorption which enhances the physical crosslinking inside the gel matrix. Besides the pH-responsive drug release features, these hydrogels are also implemented as a pulsatile drug delivery device. The electric responsive drug release behaviours are noticed and hypothesized by the formation of conducting network in the polyelectrolytic hydrogel matrix. The hydrogels are also tested as good biocompatibility and feasible cell-attachment during live-dead cell adhesion study. The drug release characteristics can also be tuned by adjusting the conducting filler loading into the gel matrix. As of our knowledge, this type of hydrogels with rubber-like consistency, high mechanical property, tunable and dual responsive drug delivery feature and very good human cell compatible is the first to report.
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Portadores de Fármacos/química , Elastómeros/química , Conductividad Eléctrica , Grafito/química , Hidrogeles/química , Fenómenos Mecánicos , Agua/química , Liberación de Fármacos , Concentración de Iones de Hidrógeno , Polimerizacion , Reología , TemperaturaRESUMEN
Carbon dots with heteroatom co-doping associated with consummate luminescence features are of acute interest in diverse applications such as biomolecule markers, chemical sensing, photovoltaic, and trace element detection. Herein, we demonstrate a straightforward, highly efficient hydrothermal dehydration technique to synthesize zinc and nitrogen co-doped multifunctional carbon dots (N, Zn-CDs) with superior quantum yield (50.8%). The luminescence property of the carbon dots can be tuned by regulating precursor ratio and surface oxidation states in the carbon dots. A unique attribution of the as-prepared carbon dots is the high monodispersity and robust excitation-independent emission behavior that is stable in enormously reactive environment and over a wide range of pH. These N, Zn-CDs unveils captivating bacteriostatic activity against gram-negative bacteria Escherichia coli. Furthermore, the excellent luminescence properties of these carbon dots were applied as a platform of sensitive biosensor for the detection of hydrogen peroxide. Under optimized conditions, these N, Zn-CDs reveals high sensitivity over a broad range of concentrations with an ultra-low limit of detection (LOD) indicating their pronounced prospective as a fluorescent probe for chemical sensing. Overall, the experimental outcomes propose that these zero-dimensional nano-dots could be developed as bacteriostatic agents to control and prevent the persistence and spreading of bacterial infections and as a fluorescent probe for hydrogen peroxide detection.
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Antibacterianos/química , Técnicas Biosensibles/métodos , Escherichia coli/crecimiento & desarrollo , Peróxido de Hidrógeno/análisis , Nitrógeno/química , Puntos Cuánticos/química , Zinc/químicaRESUMEN
Diphosphene TerMesP = PTerMes (1; TerMes = 2,6-Mes2C6H3; Mes = 2,4,6-Me3C6H2) and NHCMe42 (NHCMe4 = 1,3,4,5-tetramethylimidazol-2-ylidene) exist in an equilibrium mixture with the NHCMe4 -coordinated diphosphene 3. While uncoordinated 1 is inert to hydrolysis, the NHC adduct 3 readily undergoes hydrolysis to afford a phosphino-substituted phosphine oxide with the liberation of NHCMe4 . On this basis, conditions suitable for the catalytic use of NHCMe4 were identified. Similarly, while the hydrogenation of free diphosphene 1 with H3N·BH3 is very slow, 3 reacts instantaneously with H3N·BH3 at room temperature to afford a dihydrodiphosphane.
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Proper waste disposal from household and restaurants is becoming an important and recurring waste-management concern. Herein, a method of upcycling of waste kitchen chimney oil has been adopted to prepare fluorescent multifunctional carbon quantum dots. These nanodots showed superior biocompatibility, excellent optical properties, water solubility and high yield. Preparation of C-dots from highly abundant carbon source of waste refusals is highly effective in commercial aspect as well as in reducing the immense environmental pollution. The C-dots showed quasi-spherical size obtained from high resolution transmission electron microscopy (HRTEM) having an abundance of 1-4â¯nm in size. The ease of water dispersibility of the nanodots is a mere reflection of their surface polarity which has been supported by Fourier transformed infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). In the field of practical acceptability, the C-dots have been experimented to sense Fe3+ ion in a wide range of concentration (1â¯nM to 600⯵M) with a detection limit of 0.18â¯nM which can be termed as 'tracer metal chemosensor'. Moreover, the prepared carbon dots were also tested against inter-cellular Fe3+ ion sensing probe. Lastly, we also fabricate the biopolymercarbon dots composite for fluorescent marker ink and light emitting polymer film.
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Monitoreo del Ambiente/métodos , Compuestos Férricos/análisis , Aceites de Plantas/química , Polímeros/química , Puntos Cuánticos/química , Carbono/química , Línea Celular , Supervivencia Celular/efectos de los fármacos , Monitoreo del Ambiente/economía , Colorantes Fluorescentes/química , Humanos , Iones/química , Límite de Detección , Microscopía de Fuerza Atómica , Microscopía Fluorescente , Tamaño de la Partícula , Espectroscopía de Fotoelectrones , Puntos Cuánticos/toxicidad , Sonicación , Espectrofotometría Ultravioleta , Espectroscopía Infrarroja por Transformada de FourierRESUMEN
Sequentially prepared semi-interpenetrating polymer network (semi-IPN) has been developed here via Michael type addition of acrylic acid (AA) and 2-acrylamido-2-methylpropane sulfonic acid (AMPS) on to starch. The semi-IPN hydrogel have proficiency in fast water imbibition towards gel network and swelling tunable character with pH alteration in ambient condition. The synthesized gel has been characterized by Fourier transformed infrared spectroscopy (FTIR) to confirm Michael type grafting of monomers on to starch. The surface morphology, observed from Scanning Electron Microscopy (SEM) exhibited corrugated rough surface on hydrogel which enhances the fast water uptake feature by anomalous Fickian case II diffusion mechanism. Grafting reaction also improves its thermal stability which has been confirmed by thermogravimetric analysis (TGA). Biodegradation study with hen egg lysozyme medium reveals the accelerated enzymatic scission of the starch backbone and progressive mass loss. Degradation of the hydrogel around 60% of its primary mass has been observed within 7days. The physicochemical characterizations of this hydrogel suggest this as a promising pH-tunable, biodegradable candidate for control drug delivery vehicle.
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Portadores de Fármacos/química , Portadores de Fármacos/metabolismo , Hidrogeles/química , Memantina/química , Almidón/química , Almidón/metabolismo , Animales , Preparaciones de Acción Retardada , Difusión , Liberación de Fármacos , Estabilidad de Medicamentos , Concentración de Iones de Hidrógeno , Cinética , Temperatura , Agua/químicaRESUMEN
The emerging popularity and wide acceptance of green chemistry and environmentally benign/ecofriendly approaches have comprehensively considered for catalyst synthesis methods. Natural resource derived carbogenic quantum dots has been used in assistance with ultrasonic shock wave to graphene oxide (GO) aqueous dispersion in order to prepare reduced graphene oxide decorated with silver nanoparticles following the 'top-down' method. The total reduction process is done without using any toxic external reducing agents and any surfactants or stabilizers, thus it can be accepted as green method. Sonochemical destratification of the GO layers provides green attributes due to scalable, non-hazardous and relatively fast reduction to enhance surface area of the GO. Arresting the silver nanoparticles onto basal planes of graphene oxide can act as an efficient solid state support catalyst for fast reduction of toxic nitro aryls. Besides this work also reports bactericidal feature exhibited by the catalyst. Thus a dual functioning nanomaterial has been successfully developed which can be a suitable alternative for reductive forthcoming specialty/multifunctional membrane and other high-end medicinal or industrial applications.
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Antibacterianos/química , Antibacterianos/farmacología , Grafito/química , Nanopartículas del Metal/química , Óxidos/química , Plata/química , Ondas Ultrasónicas , Catálisis , Escherichia coli/efectos de los fármacos , Escherichia coli/crecimiento & desarrollo , Tecnología Química Verde , Cinética , Modelos Moleculares , Conformación Molecular , Nanotecnología , Oxidación-ReducciónRESUMEN
Zero-dimensional fluorescent nanoparticles having specificity as molecular probe appears to be strategically balanced fluorescent nano-probes. In this work, purified lemon extract and l-arginine have been thermally coupled for the extremely acute detection of Cu2+ in aqueous medium. The Cu2+ ions may be captured by the amino groups on the surface of the nano-sensor to form cupric ammine complex resulting in quenched fluorescence via an inner filter effect. Our proposed nano-probe is N-doped carbon dots (NCDs) which are efficiently selective as fluorescent chemosensor due to enormous binding affinity towards Cu2+ in a wide range of concentration (0.05-300µM) within a few minutes.