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Bradyarrhythmia poses a serious threat to human health, with chronic progression causing heart failure and acute onset leading to sudden death. In this study, we develop a scalable drug-mimicking nanoplasmonic therapeutic strategy by introducing gold nanorod (Au NR) mediated near-infrared (NIR) photothermal effects. An integrated sensing and regulation platform is established for in situ synchronized NIR laser regulation and electrophysiological property recording. The Au NR plasmonic regulation enables the restoration of normal cardiomyocyte rhythm from the bradyarrhythmia. By regulating the aspect ratio and concentration of Au NRs, as well as the intensity and time of NIR irradiation, we precisely optimized the plasmonic photothermal effect to explore effective therapeutic strategies. Furthermore, mRNA sequencing revealed a significant increase in the number of differentially expressed genes (DEGs) involved in the electrophysiological activities of cardiomyocytes following photothermal therapy. Au NR-mediated plasmonic photothermal therapy, as an efficient and noninvasive approach to bradyarrhythmia, holds profound implications for cardiology research.
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Anisotropic nanocrystals such as nanorods (NRs) display unique linearly polarized emission, which is expected to break the external quantum efficiency (EQE) limit of quantum dot-based light-emitting diodes (LEDs). However, the progress in achieving a higher EQE using NRs encounters several challenges, primarily involving a low photoluminescence quantum yield (PLQY) of NRs and imbalanced charge injection in NR-LEDs. In this work, we investigated NR-LEDs based on CdSe/CdZnS/ZnS rod-in-rod NRs with a high PLQY and higher linear polarization compared to those of dot-in-rod NRs. The balanced charge injection is achieved using ZnMgO nanoparticles as the electron transport layer and poly-TPD {poly[N,N'-bis(4-butylphenyl)-N,N'-bis(phenyl)benzidine]} as the hole transport layer. Therefore, the NR-LEDs exhibit a maximum EQE of 21.5% and a maximum luminance of >120â¯000 cd/m2 owing to the high level of in-plane transitions with a dipole moment of 90%. The NR-LEDs also have greatly inhibited droop in EQE under a high current density as well as outstanding operation lifetime and cycle stability.
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Integrating more than one type of metal into a nanoparticle that has a well-defined morphology and composition expands the functionalities of nanocatalysts. For a metal core/porous multimetallic shell nanoparticle, the availability of catalytically active surface sites and molecular mass transport can be enhanced, and the multielemental synergy can facilitate intraparticle charge transport. In this work, a reliable and robust synthesis of such a functional tetrametallic nanoparticle type is presented, where a micro- and mesoporous PdPtIr shell is grown on Au nanorods. The effect of critical synthesis parameters, namely temperature and the addition of HCl are investigated on the hydrodynamic size of the micellar pore template as well as on the stability of the metal chloride complexes and various elemental analysis techniques prove composition of the porous multimetallic shell. Due to the synergistic properties, the tetrametallic nanorods possess extensive negative surface charge making them a promising catalyst in reduction reactions. Dye degradation as well as the conversion of p-nitrophenol to p-aminophenol is catalyzed by the supportless nanorods without light illumination. By depositing the particles onto conductive substrates, the nanostructured electrodes show promising electrocatalytic activity in ethanol oxidation reaction. The nanocatalyst presents excellent morphological stability during all the catalytic test reactions.
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Semiconducting nanocrystals have attracted world-wide research interest in artificial photosynthesis due to their appealing properties and enticing potentials in converting solar energy into valuable chemicals. Compared to 0D nanoparticles, 1D nanorods afford long-distance charge carriers separation and extended charge carriers lifetime due to the release of quantum confinement in axial direction. Herein, stable CsPbBr3 nanorods of distinctive dimensions are crafted without altering their properties and morphology via grafting hydrophobic polystyrene (PS) chains through a post-synthesis ligand exchange process. The resulting PS-capped CsPbBr3 nanorods exhibit a series of enhanced stabilities against UV irradiation, elevated temperature, and polar solvent, making them promising candidates for photo-induced atom transfer radical polymerization (ATRP). Tailoring the surface chemistry and dimension of the PS-capped CsPbBr3 nanorods endows stable, but variable reaction kinetics in the photo-induced ATRP of methyl methacrylate. The trapping-detrapping process of photogenerated charge carriers lead to extended lifetime of charge carriers in lengthened CsPbBr3 nanorods, contributing to a facilitated reaction kinetics of photo-induced ATRP. Therefore, by leveraging such stable PS-capped CsPbBr3 nanorods, the effects of surface chemistry and charge carriers dynamics on its photocatalytic performance are scrutinized, providing fundamental understandings for designing next-generation efficient nanostructured photocatalyst in artificial photosynthesis and solar energy conversion.
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Bone matrix exhibits exceptional mechanical properties due to its unique nanocomposite structure of type I collagen fibrils and hydroxyapatite (HAp) nanoparticles in hierarchical liquid crystalline (LC) order. However, the regeneration mechanism of this LC structure is elusive. This study investigates the role of the LC structure of HAp nanorods in guiding aligned mineralization and its underlying molecular mechanism. A unidirectionally oriented LC phase of HAp nanorods is developed through engineering-assisted self-assembling. This is used to study the growth direction of long-range aligned extracellular matrix (ECM) and calcium deposit formation during the osteogenic differentiation of human bone marrow-derived mesenchymal stem cells. It is found that 2 key regulatory genes, COL1A1 and COL4A6, lead to the formation of aligned ECM. Activation of the PI3K-Akt pathway enhances osteogenesis and promotes ordered calcium deposits. This study provides evidence for elucidating the mechanism of LC-induced ordered calcium deposition at hierarchical levels spanning from the molecular to macro-scale, as well as the switch from ordered to disordered mineralization. These findings illuminate bone regeneration, contribute to the development of biomimetic artificial bone with long-range ordered structures, and suggest a basis for therapeutic targeting of microstructure-affected bone disorders and the broader field of cell-ECM interactions.
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Nanostructured metal hydrides with unique morphology and improved hydrogen storage properties have attracted intense interests. However, the study of the growth process of highly active borohydrides remains challenging. Herein, for the first time the synthesis of LiBH4 nanorods through a hydrogen-assisted one-pot solvothermal reaction is reported. Reaction of n-butyl lithium with triethylamine borane in n-hexane under 50 bar of H2 at 40-100 °C gives rise to the formation of the [100]-oriented LiBH4 nanorods with 500-800 nm in diameter, whose growth is driven by orientated attachment and ligand adsorption. The unique morphology enables the LiBH4 nanorods to release hydrogen from ≈184 °C, 94 °C lower than the commercial sample (≈278 °C). Hydrogen release amounts to 13 wt% within 40 min at 450 °C with a stable cyclability, remarkably superior to the commercial LiBH4 (≈9.1 wt%). More importantly, up to 180 °C reduction in the onset temperature of hydrogenation is successfully attained by the nanorod sample with respect to the commercial counterpart. The LiBH4 nanorods show no foaming during dehydrogenation, which improves the hydrogen cycling performance. The new approach will shed light on the preparation of nanostructured metal borohydrides as advanced functional materials.
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High-precision, controllable, mass-producible assembly of nanoparticles into complex structures or devices holds immense importance in the application across various fields but it remains challenging. Here a highly controllable and reversible active assembly of colloidal CsPbBr3 nanorods, driven by an external electric field is achieved. This approach enables the nanorods dynamically orient themselves, assemble into chains, aggregate into columns, and eventually form an ordered column array, with the electric field intensity varying from 0 to 50 V µm-1 at 100 kHz. The nanorods inside the columns align parallel to the electric field, leading to a well-ordered structure. With the analysis of the interactions among the nanorods, a quantitative interpretation of the assembly is proposed. Monte Carlo calculation is also introduced to simulate the assembly process and the results prove to be in great agreement with the experimental observations. This electric field-driven assembly presents an exciting opportunity to pave the way for next-generation sensors and photonic devices based on well-developed colloidal nanoparticles.
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Here, elongated pseudohollow nanoframes composed of four rectangular plates enclosing the sides and two open-frame ends with four ridges pointing at the tips for near-field focusing are reported. The side facets act as light-collecting domains and transfer the collected light to the sharp tips for near-field focusing. The nanoframes are hollow inside, allowing the gaseous analyte to penetrate through the entire architecture and enabling efficient detection of gaseous analytes when combined with Raman spectroscopy. The resulting nanostructures are named Au dodecahedral-walled nanoframes. Synthesis of the nanoframes involves shape transformation of Au nanorods with round tips to produce Au-elongated dodecahedra, followed by facet-selective Pt growth, etching of the inner Au, and regrowth steps. The close-packed assembly of Au dodecahedral-walled nanoframes exhibits an attomolar limit of detection toward benzenethiol. This significant enhancement in SERS is attributed to the presence of a flat solid terrace for a large surface area, sharp edges and vertices for strong electromagnetic near-field collection, and open frames for effective analyte transport and capture. Moreover, nanoframes are applied to detect chemical warfare agents, specifically mustard gas simulants, and 20 times higher sensitivity is achieved compared to their solid counterparts.
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Caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), coronavirus disease 2019 (COVID-19) has shown extensive lung manifestations in vulnerable individuals, putting lung imaging and monitoring at the forefront of early detection and treatment. Magnetic particle imaging (MPI) is an imaging modality, which can bring excellent contrast, sensitivity, and signal-to-noise ratios to lung imaging for the development of new theranostic approaches for respiratory diseases. Advances in MPI tracers would offer additional improvements and increase the potential for clinical translation of MPI. Here, a high-performance nanotracer based on shape anisotropy of magnetic nanoparticles is developed and its use in MPI imaging of the lung is demonstrated. Shape anisotropy proves to be a critical parameter for increasing signal intensity and resolution and exceeding those properties of conventional spherical nanoparticles. The 0D nanoparticles exhibit a 2-fold increase, while the 1D nanorods have a > 5-fold increase in signal intensity when compared to VivoTrax. Newly designed 1D nanorods displayed high signal intensities and excellent resolution in lung images. A spatiotemporal lung imaging study in mice revealed that this tracer offers new opportunities for monitoring disease and guiding intervention.
Assuntos
Nanopartículas de Magnetita , Nanopartículas , Camundongos , Animais , Anisotropia , Diagnóstico por Imagem/métodos , Magnetismo , Fenômenos Magnéticos , Imageamento por Ressonância MagnéticaRESUMO
As opposed to natural photosynthesis, a significant challenge in a semiconductor-based photocatalyst is the limited hole extraction efficiency, which adversely affects solar-to-fuel efficiency. Recent studies have demonstrated that photocatalysts featuring spatially isolated dual catalytic oxidation/reduction sites can yield enhanced hole extraction efficiencies. However, the decay dynamics of excited states in such photocatalysts have not been explored. Here a ternary barbell-shaped CdS/MoS2/Cu2S heterostructure is prepared, comprising CdS nanorods (NRs) interfaced with MoS2 nanosheets at both ends and Cu2S nanoparticles on the sidewall. By using transient absorption (TA) spectra, highly efficient charge separation within the CdS/MoS2/Cu2S heterostructure are identified. This is achieved through directed electron transfer to the MoS2 tips at a rate constant of >8.3 × 109 s-1 and rapid hole transfer to the Cu2S nanoparticles on the sidewall at a rate of >6.1 × 1010 s-1, leading to an exceptional overall charge transfer constant of 2.3 × 1011 s-1 in CdS/MoS2/Cu2S. The enhanced hole transfer efficiency results in a remarkably prolonged charge-separated state, facilitating efficient electron accumulation within the MoS2 tips. Consequently, the ternary CdS/MoS2/Cu2S heterostructure demonstrates a 22-fold enhancement in visible-light-driven H2 generation compare to pure CdS nanorods. This work highlights the significance of efficient hole extraction in enhancing the solar-to-H2 performance of semiconductor-based heterostructure.
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Energy-efficient white light-emitting diodes (LEDs) are in high demand across the society. Despite the significant advancements in the modern lighting industry based on solid-state electronics and inorganic phosphor, solid-state lighting (SSL) continues to pursue improved efficiency, saturated color performance, and longer lifetime. Here in this article, robust, narrow emission band nanorods (NRs) are disclosed with tailored wavelengths, aiming to enhance the color rendering index (CRI) and luminous efficacy (LE). The fabricated lighting device consists of NRs of configuration CdSe/ZnxCd1-xS/ZnS, which can independently tune CRI R1-R9 values and maximize the luminous efficacy. For general lighting, NRs with quantum yield (QY) up to 96% and 99% are developed, resulting in ultra-efficient LEDs reaching a record high luminous efficacy of 214 lm W-1 (certified by the National Accreditation Service). Furthermore, NRs are deployed onto mid-power (0.3 W@ 50 mA) LEDs, showing significantly enhanced long-term stability (T95 = 400 h @ 50 mA). With these astonishing properties, the proposed NRs can pave the way for efficient lighting with desired optical spectrum.
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Anode materials for sodium ion batteries (SIBs) are confronted with severe volume expansion and poor electrical conductivity. Construction of assembled structures featuring hollow interior and carbon material modification is considered as an efficient strategy to address the issues. Herein, a novel template-assisted epitaxial growth method, ingeniously exploiting lattice matching nature, is developed to fabricate hollow ordered architectures assembled by SnO2 nanorods. SnO2 nanorods growing along [100] direction can achieve lattice-matched epitaxial growth on (110) plane of α-Fe2O3. Driven by the lattice matching, different α-Fe2O3 templates possessing different crystal plane orientations enable distinct assembly modes of SnO2, and four kinds of hollow ordered SnO2@C nanorods arrays (HONAs) with different morphologies including disc, hexahedron, dodecahedron and tetrakaidecahedron (denoted as Di-, He-, Do-, and Te-SnO2@C) are achieved. Benefiting from the synergy of hollow structure, carbon coating and ordered assembly structure, good structural integrity and stability and enhanced electrical conductivity are realized, resulting in impressive sodium storage performances when utilized as SIB anodes. Specifically, Te-SnO2@C HONAs exhibit excellent rate capability (385.6 mAh·g-1 at 2.0 A·g-1) and remarkable cycling stability (355.4 mAh·g-1 after 2000 cycles at 1.0 A·g-1). This work provides a promising route for constructing advanced SIB anode materials through epitaxial growth for rational structural design.
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Solar-blind ultraviolet (SBUV) to near-infrared (NIR) broadband photodetectors (BB-PD) have important applications in environmental monitoring and other applications. However, it is challenging to prepare SBUV-IR photosensitive materials via simple steps and to construct SBUV-IR broadband devices for multiplex detection with high sensitivity at different wavelengths. Here, self-powered and broadband photodetectors using a high-performance mixed dimensional Sb2O3 nanorod 1-dimension (1D)/monodisperse microdiamond-like PdTe2 3-dimension (3D)/Si (3D) heterojunction for multiplex detection of environmental pollutants with high sensitivity at broadband wavelength are developed. The 1D/3D mixed dimensional Sb2O3/PdTe2/Si structure combines the advantages of strong light absorption, high carrier transport efficiency of 1D Sb2O3 nanorods, and expansion of interface barrier caused by 3D microdiamond-like PdTe2 interlayer to improve the photocurrent density and self-powered ability. The efficient photogenerated charge separation enables anon/off ratio of more than 5 × 106. The device exhibits excellent photoelectric properties from 255 to 980 nm with the responsivity from 4.56 × 10-2 to 6.55 × 10-1 AW-1, the detectivity from 2.36 × 1012 to 3.39 × 1013 Jones, and the sensitivity from 3.90 × 107 to 1.10 × 1010 cm2 W-1 without external bias. Finally, the proposed device is applied for the multiplex monitoring of environmental pollution gases NO2 with the detection limit of 200 ppb and PM2.5 particles at mild pollution at broadband wavelength. The proposed BB-PD has great potential for multiplex detection of environmental pollutants and other analytes at broadband wavelength.
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The conversion of CO2 into valuable solar fuels via photocatalysis is a promising strategy for addressing energy shortages and environmental crises. Here, novel In2 O3 @Co2 VO4 hierarchical heterostructures are fabricated by in situ growing Co2 VO4 nanorods onto In2 O3 nanofibers. First-principle calculations and X-ray photoelectron spectroscopy (XPS) measurements reveal the electron transfer between In2 O3 and Co2 VO4 driven by the difference in work functions, thus creating an interfacial electric field and bending the bands at the interfaces. In this case, the photogenerated electrons in In2 O3 transport to Co2 VO4 and recombine with its holes, indicating the formation of In2 O3 @Co2 VO4 S-scheme heterojunctions and resulting in effective separation of charge carriers, as confirmed by in situ irradiation XPS. The unique S-scheme mechanism, along with the enhanced optical absorption and the lower Gibbs free energy change for the production of * CHO, significantly contributes to the efficient CO2 photoreduction into CO and CH4 in the absence of any molecule cocatalyst or scavenger. Density functional theory simulation and in situ diffuse reflectance infrared Fourier transform spectroscopy are employed to elucidate the reaction mechanism in detail.
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Halide perovskite, renowned for its multifunctional properties, shows considerable promise for realizing self-charging power systems. In this study, a lead-free methylammonium bismuth iodide (MA3Bi2I9) perovskite is used to create a self-charging power unit (SPU). This involves constructing a hybrid piezoelectric-triboelectric nanogenerator (Hybrid-TENG) and utilizing MA3Bi2I9 for energy storage as an anode in a lithium-ion battery (LIB). Initially, MA3Bi2I9 nanorods are synthesized and composited with a polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene polymer. The dielectric and mechanical properties of composite films having perovskite loading content are investigated. The optimized Hybrid-TENG exhibits superior performance, generating a voltage of 537 V, current density of 13.2 µA cm- 2, and maximum power density of 3.04 mW cm-2, which can be attributed to the high piezoelectric coefficient of MA3Bi2I9 nanorods (≈20.6 pm V-1). A MA3Bi2I9 thin film, serving as an electrode in LIB, demonstrates a high specific capacity of 2378.9 mAh cm-3 (578.8 mAh g-1) with a capacity retention of ≈87.5% over 100 cycles, underscoring its stable performance. Furthermore, a Hybrid-TENG is employed to charge the MA3Bi2I9-based LIB, thus realizing an SPU for driving portable electronics. This study highlights the promising potential of perovskites for developing efficient nanogenerators and LIBs, paving the way for sustainable energy solutions in small-scale electronics.
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Temperature-modulated colloidal phase of plasmonic nanoparticles is a convenient playground for resettable soft-actuators or colorimetric sensors. To render reversible clustering under temperature change, bulky ligands are required, especially if anisotropic morphologies are of interest. This study showcases thermoresponsive gold nanorods by employing small surface ligands, bis (p-sulfonatophenyl) phenyl-phosphine dihydrate dipotassium salt (BSPP) and native cationic surfactant. Temperature-dependent analysis in real-time allowed to describe the structural features (interparticle distance and cluster size) as well as thermal parameters, melting and freezing temperatures. These findings suggest that neither covalent Au-S bonds nor bulky ligands are required to obtain a robust thermoresponsive system based on anisotropic gold nanoparticles, paving the way to stimuli-responsive nanoparticles with a wide range of sizes and geometries.
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As a potential candidate for photocatalytic H2 production from water splitting, Ta2O5 catalyst presents suitable conduction and valence band positions, but suffers from poor charge transfer ability, which seriously limits its photocatalytic performance enhancement. Here, a facile and eco-friendly hydrothermal method was developed for the fabrication of one-dimensional (1D) Ta2O5 nanorods using the freshly precipitated tantalic acids as the precursors. An oriented attachment mechanism was proposed for the growth of Ta2O5 nanorods. Moreover, the present synthetic approach was further extended to direct synthesis of nine kinds of alkaline tantalates and alkaline-earth tantalates nanostructures, suggesting its general applicability. A significant increase in activity in photocatalytic H2 production was revealed on 1D Ta2O5 nanorods. The improved photocatalytic H2 production activity of Ta2O5 nanorods was mainly attributed to its 1D nanorods structure with high crystallization and large speciï¬c surface areas as well as excellent charge transfer efficiency.
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Gold nanorods (AuNRs) have attracted significant attention over the past several decades for a variety of applications and there has been steady progress with regards to their synthesis and modification. Despite these advances, the assembly of AuNRs into well-organized hierarchical assemblies remains a formidable challenge. Specifically, there is a need for tools that can fabricate assemblies of nanorods over large length scales at low cost with the potential for high-throughput manufacturing. Langmuir-Blodgettry is a monolayer deposition technique which has been primarily applied to amphiphilic molecules, but which has recently shown promise for the ordering of functionalized nanoparticles residing at the air-water interface. In this work, Langmuir-Blodgett deposition is explored for the formation of AuNR arrays for enhanced surface-enhanced Raman spectroscopy (SERS) sensing. In particular, both surface modification of the AuNRs as well as subphase modification with cysteamine were evaluated for AuNR array fabrication.
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Transition metal oxides are investigated as electrochemically active anodes for several years due to the merits of high specific capacity, low cost, abundant resources and controllable synthesis. But the poor cycle performances have hindered their further wide application. Herein, porous La-doped FeOOH nanorods have been synthesized through a facile hydrothermal method, which could be transformed into porous La-doped Fe2O3 (Fe2O3-La) via a simple heating process. Compared with the undoped Fe2O3, the Fe2O3-La showed larger surface area, higher specific capacities and more stable cycle performances for lithium/sodium ion batteries. In addition, as an advanced sulfur host for lithium-sulfur batteries, the Fe2O3-La also displayed much more excellent cycle and rate performances than the undoped Fe2O3. The superior electrochemical performances of the Fe2O3-La may could be attributed to the doping of La, which could induce more porous morphology and offer more reactive sites. The positive effects of La-doping for electrochemical performances of porous Fe2O3 nanorods provide novel insights for further applications of rare earth metal doping.
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In the framework of the design, synthesis and testing of a library of copper complexes and nanostructured assemblies potentially endowed with antitumor and antiviral activity and useful for several applications, from drugs and related delivery systems to the development of biocidal nanomaterials, we present the detailed spectroscopic investigation of the molecular and electronic structure of copper-based coordination compounds and of a new conjugated system obtained by grafting Cu(I) complexes to gold nanorods. More in detail, the electronic and molecular structures of two Cu complexes and one AuNRs/Cu-complex adduct were investigated by X-ray photoelectron spectroscopy (XPS), synchrotron-induced XPS (SR-XPS) and near edge X-ray absorption spectroscopy (NEXAFS) in solid state, and the local structure around copper ion was assessed by X-ray absorption spectroscopy (XAS) both in solid state and water solution for the AuNRs/Cu-complex nanoparticles. The proposed multi-technique approach allowed to properly define the coordination geometry around the copper ion, as well as to ascertain the molecular structures of the coordination compounds, their stability and modifications upon interaction with gold nanoparticles, by comparing solid state and liquid phase data.