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Lattice Strain Formation through Spin‐Coupled Shells of MoS <sub/>2</sub> on Mo <sub/>2</sub> C for Bifunctional Oxygen Reduction and Oxygen Evolution Reaction Electrocatalysts
摘要： Identifying effective means to improve the electrocatalytic performance of transition metal dichalcogenides in alkaline electrolytes is a significant challenge. Herein, an advanced electrocatalyst possessing shells of molybdenum disulfide (MoS2) on molybdenum carbide (Mo2C) for efficient electrocatalytic activity in alkaline electrolytes is reported. The strained sheets of curved MoS2 surround the surface of Mo2C, turning the inactive basal planes of MoS2 into highly active electrocatalytic sites in the alkaline electrolyte. The van der Waals layers, which even possess van der Waals epitaxy along (100) facets of MoS2 and Mo2C, enhance the spin coupling between MoS2 and Mo2C, providing an easy electron transfer path for excellent electrocatalytic activity in alkaline electrolytes and solving the stability issue. In addition, it is found that curved MoS2 sheets on Mo2C show 3.45% tensile strain in the lattice, producing excellent catalytic activity for both oxygen reduction reaction (ORR) (with E1/2 = 0.60 V vs RHE) and oxygen evolution reaction (OER) (overpotential = 1.51 V vs RHE at 10 mA cm?2) with 60 times higher electrochemical active area than pristine MoS2. The unique structure and synthesis route outlined here provide a novel and efficient approach toward designing highly active, durable, and cost-effective ORR and OER electrocatalysts.
关键词： bifunctional,spin coupled,core–shell structures,oxygen electrocatalysis,lattice strain
更新于2025-09-11 14:15:04
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European Microscopy Congress 2016: Proceedings || SEM based electro-optical characterization of core-shell LEDs and simulation of imaging including CL and EBIC excitation inside ensembles
摘要： Three dimensional (3D) nano- and microstructures (NAMs) are attracting a lot of attention and are discussed regarding several applications, especially in optoelectronics and sensors. For example GaN based 3D light emitting diodes (LEDs) with a core-shell geometry are supposed to have substantial advantages over conventional planar LEDs: The active area along the sidewalls of hexagonal GaN pillars can considerably be increased by high aspect ratios - leading to a lower current density inside the InGaN quantum well (QW) at the same operation current per substrate area. [1] Thus related methods are requested for characterization of local electro-optical properties with a high spatial resolution on single structures as well as in ensembles. Usually, electron microscopy is employed to investigate the geometry and properties of such 3D-NAMs and for mapping of vertical features by an SEM a certain sample tilt (e.g. about 30°) is needed. Investigation of single 3D-LEDs by electron beam induced current (EBIC) using an SEM based manipulator setup proves the presence of a pn-junction and doping type of the core and shell, while cathodoluminescence (CL) gives an insight to the optical properties of the QW [2]. But in contrast to SEM on planar regions the interactions of the electron probe are significantly affected by the 3D geometry and the surrounding of the NAMs. In ensembles of 3D-NAMs a certain portion of incident electrons are scattered into neighbor structures and conventional SEM signals (SE, BSE, CL, X-ray emission) are partly shadowed. This interaction is affecting the SEM imaging contrast and the probed signal also includes contributions which are not related to the material properties at the electron beam spot. As such parasitic signals are generated quite close to the original region of the interaction most (global) SEM detectors cannot separate them from the original source. In particular scattering events occur in an enlarged volume of the sample (of the substrate and NAMs) leading to a reduced excitation density and parasitic effects, e.g. this causes a significant contribution of defect related yellow luminescence (YL) We present results of InGaN/GaN core-shell LEDs obtained with an FE-SEM which is equipped with SE, In-Beam SE, low-kV BSE, EBIC and monochromatic CL detection as well as a piezo controlled manipulator setup, see Figure 1. A modified parabolic collection mirror enables measuring luminescence from planar samples up to 4’’ in a tilted view up to 30°. For a quantitative interpretation of CL and EBIC measurement values and image contrasts, the physical modeling of SEM images and spatially resolved energy transfer by a probe spot is necessary. This is performed using the simulation program MCSEM [3]. It models the different stages of image formation and generates SEM images of complex NAM shapes using e.g. GaN as model material. Aspects of the simulation are the electron probe formation, a 3D model of the specimen structure, the interaction of electron probe and solid state by means of scattering trajectories, the emission of secondary electrons, and different types of electron detectors, see Figure 2 and Figure 3. An insight to CL and EBIC imaging is gained by evaluating the scattering energy deposited in a distinct volume inside the NAMs as an imaging signal - this is related to the generation rate of electron-hole pairs inside the respective volume of the semiconductor. Consent to the experiments this simulation reveals an edge contrast and shadowing of signals by the ensemble as well as scattering of primary electrons inside the ensemble of 3D-NAMs. A quantitative comparison is possible by the absorbed current (EBAC). Artefacts of the EBIC are also demonstrated by the simulation, in particular edge contrast by a reduced generation rate and parasitic signals by scattering from neighbor structures.
关键词： EBIC,cathodoluminescence,electron beam induced current,SEM simulation,core-shell LED
更新于2025-09-11 14:15:04
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Electrochemically controlled CdS@CdSe nanoparticles on ITO@TiO2 dual core-shell nanowires for enhanced photoelectrochemical hydrogen production
摘要： Here, we report a novel dual heterostructured photoanode consisting of CdS@CdSe core-shell nanoparticles (NPs) and 1D-structure tin-doped indium oxide (ITO)@TiO2 core-shell nanowires (ITO@TiO2@CdS@CdSe) for highly efficient photoelectrochemical (PEC) hydrogen production. The finely controlled hierarchical core-shell CdS@CdSe sensitization from consecutive electrochemical deposition on the ITO@TiO2 core-shell nanowire has synergistic effects of visible-light utilization and efficient charge transport on the PEC response. The rationally designed dual core-shell heterostructure leads to cascade charge migration throughout the aligned energy band edges with rapid charge extraction through the hierarchical heterostructure of ITO@TiO2@CdS@CdSe, alleviating the crucial charge accumulation. As a result, the dual heterostructured photoanode exhibits a maximum photocurrent density of 20.11 mA/cm2 at 1.23 V vs. the reversible hydrogen electrode (RHE) and a dramatic enhancement in the incident photon-to-current efficiency (IPCE) over the extended absorption spectrum. The time-resolved photoluminescence (TRPL) characterization indicates the realized multiple-band cascade charge migration throughout ITO@TiO2@CdS@CdSe could promote an 8-fold increase in the charge separation efficiency. This rational design of dual-heterojunction-structured photoelectrodes via electrochemical deposition provides a demonstration of modifying conventional light-harvesting photoelectrodes with stagnate solar energy conversion and PEC hydrogen production.
关键词： cascade charge transport,solar hydrogen production,electrochemical core-shell deposition,photoelectrochemical cell,dual heterostructure
更新于2025-09-11 14:15:04
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A novel approach to coat silica on quantum dots: Forcing decomposition of tetraethyl orthosilicate in toluene at high temperature
摘要： The coating of silica (SiO2) on quantum dots (QDs) has been widely studied, because SiO2 can protect QDs from the damages of moisture, radiation, and heat. Conventional SiO2 coating methods for QDs are usually performed in aqueous or emulsion solutions, which require the addition of water for the hydrolysis of SiO2 precursors and lead to the photoluminescence (PL) quenching of QDs. To address this issue, a novel SiO2 coating approach on single particle level was developed by the thermally forcing decomposition of tetraethyl orthosilicate in toluene. The CdSe/CdS/ZnS:Al@SiO2 nanoparticles (NPs) were prepared without decreasing the original PL quantum yield (QY), which exhibited much better photo and thermal stability in comparison with uncoated CdSe/CdS/ZnS:Al QDs. Furthermore, due to the natural formation of silanol groups on the SiO2 shell, CdSe/CdS/ZnS:Al@SiO2 NPs present not only good solubility but also excellent room temperature stability in phosphate buffer saline solution for several months.
关键词： SiO2,TEOS,stability,core/shell quantum dots,water solubility
更新于2025-09-11 14:15:04
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Effects of Zn <sup>2+</sup> and Ga <sup>3+</sup> doping on the quantum yield of cluster-derived InP quantum dots
摘要： As the commercial display market grows, the demand for low-toxicity, highly emissive, and size-tunable semiconducting nanoparticles has increased. Indium phosphide quantum dots represent a promising solution to these challenges; unfortunately, they typically suffer from low inherent emissivity resulting from charge carrier trapping. Strategies to improve the emissive characteristics of indium phosphide often involve zinc incorporation into or onto the core itself and the fabrication of core/shell heterostructures. InP clusters are high fidelity platforms for studying processes such as cation exchange and surface doping with exogenous ions since these clusters are used as single-source precursors for quantum dot synthesis. Here, we examined the incorporation of zinc and gallium ions in InP clusters and the use of the resultant doped clusters as single-source precursors to emissive heterostructured nanoparticles. Zinc ions were observed to readily react with InP clusters, resulting in partial cation exchange, whereas gallium resisted cluster incorporation. Zinc-doped clusters effectively converted to emissive nanoparticles, with quantum yields strongly correlated with zinc content. On the other hand, gallium-doped clusters failed to demonstrate improvements in quantum dot emission. These results indicate stark differences in the mechanisms associated with aliovalent and isovalent doping and provide insight into the use of doped clusters to make emissive quantum dots.
关键词： Indium phosphide,core/shell heterostructures,quantum yield,gallium doping,quantum dots,zinc doping
更新于2025-09-11 14:15:04
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Nanostructured colloidal quantum dots for efficient electroluminescence devices
摘要： The exceptional quality of light generated from colloidal quantum dots has attracted continued interest from the display and lighting industry, leading to the development of commercial quantum dot displays based on the photoluminescence down-conversion process. Beyond this technical level, quantum dots are being introduced as emissive materials in electroluminescence devices (or quantum dot-based light-emitting diodes), which boast high internal quantum efficiency of up to 100%, energy efficiency, thinness, and flexibility. In this review, we revisit various milestone studies regarding the core/shell heterostructures of colloidal quantum dots from the viewpoint of electroluminescence materials. Development of nanostructured colloidal quantum dots advanced from core/shell heterostructure, core/thick shell formulation, and delicate control of confinement potential shape has demonstrated close correlation of the photophysical properties of quantum dots with the performance of electroluminescence device, which provided useful guidelines on the heterostructured quantum dots for mitigating or eliminating efficiency limiting phenomena in quantum dot light emitting diodes. To enable practical and high performance quantum dot-based electroluminescence devices in the future, integration of design concepts on the heterostructures with environmentally benign systems will be crucial.
关键词： Electroluminescence,Nanocrystals,Colloidal Quantum Dots,Core/Shell Heterostructures,Light Emitting Diodes
更新于2025-09-11 14:15:04
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Towards rational design and optimization of near-field enhancement and spectral tunability of hybrid core-shell plasmonic nanoprobes
摘要： In biology, sensing is a major driver of discovery. A principal challenge is to create a palette of probes that offer near single-molecule sensitivity and simultaneously enable multiplexed sensing and imaging in the “tissue-transparent” near-infrared region. Surface-enhanced Raman scattering and metal-enhanced fluorescence have shown substantial promise in addressing this need. Here, we theorize a rational design and optimization strategy to generate nanostructured probes that combine distinct plasmonic materials sandwiching a dielectric layer in a multilayer core shell configuration. The lower energy resonance peak in this multi-resonant construct is found to be highly tunable from visible to the near-IR region. Such a configuration also allows substantially higher near-field enhancement, compared to a classical core-shell nanoparticle that possesses a single metallic shell, by exploiting the differential coupling between the two core-shell interfaces. Combining such structures in a dimer configuration, which remains largely unexplored at this time, offers significant opportunities not only for near-field enhancement but also for multiplexed sensing via the (otherwise unavailable) higher order resonance modes. Together, these theoretical calculations open the door for employing such hybrid multi-layered structures, which combine facile spectral tunability with ultrahigh sensitivity, for biomolecular sensing.
关键词： plasmonic nanoprobes,near-field enhancement,hybrid core-shell,biomolecular sensing,spectral tunability,multiplexed sensing
更新于2025-09-11 14:15:04
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A Review on Improving the Quality of Perovskite Films in Perovskite Solar Cells via the Weak Forces Induced by Additives
摘要： It is a challenge to design intelligent thermal metamaterials due to the lack of suitable theories. Here we propose a kind of intelligent thermal metamaterials by investigating a core-shell structure, where both the core and shell have an anisotropic thermal conductivity. We solve Laplace’s equation for deriving the equivalent thermal conductivity of the core-shell structure. Amazingly, the solution gives two coupling relations of conductivity tensors between the core and the shell, which cause the whole core-shell structure to counterintuitively self-?x a constant isotropic conductivity even when the area or volume fraction of the core changes within the full range in two or three dimensions. The theoretical ?ndings on fraction-independent properties are in sharp contrast with those predicted by the well-known e?ective medium theories, and they are further con?rmed by our laboratory experiments and computer simulations. This work o?ers two coupling relations for designing intelligent thermal metamaterials, and they are not only helpful for thermal stabilization or camou?age/illusion, but they also o?er hints on how to achieve similar metamaterials in other ?elds.
关键词： Laplace’s equation,intelligent thermal metamaterials,core-shell structure,anisotropic thermal conductivity,self-fixing behavior
更新于2025-09-11 14:15:04
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Improved performance of solution processed organic solar cells with an additive layer of sol-gel synthesized ZnO/CuO core/shell nanoparticles
摘要： In this study, ZnO/CuO core/shell nanoparticles with ZnO:CuO molar ratios of 1:1 M, 1:2 M and 2:1M were successfully synthesized via sol-gel method. The synthesized nanoparticles were characterized to investigate for their morphology, structure, purity and optical properties. XRD analysis confirmed that the synthesized particles are in nanometer range with average particle size less than 100 nm and was further verified by TEM analysis. SEM images revealed spherical shape of nanoparticles. EDX analysis confirmed the purity of nanoparticles. Near band edge emission and broad green band was recorded in the PL spectra. The bandgap of synthesized nanoparticles was observed in the range 3.85-3.91 eV. Furthermore, the effect of adding an extra active layer of ZnO/CuO core/shell nanoparticles on the performance of organic solar cell with photo active layer electron donor poly(3- hexylthiophene-2,5-diyl) (P3HT) and electron acceptor [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) was studied. Results showed that the added inorganic layer improved the absorption in visible region with increase in surface roughness of the active layer. The power conversion efficiency (PCE) shows improvement by inclusion of inorganic layer prior to organic active layer blend. This increase in PCE was basically due to increase in Voc, Jsc and FF of the fabricated device.
关键词： solar cell,Core/shell,sol-gel,ZnO/CuO,nanoparticles
更新于2025-09-11 14:15:04
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Carbon coated TiO2 nanoparticles prepared by pulsed laser ablation in liquid, gaseous and supercritical CO2
摘要： We report on the synthesis of TiO2 nanoparticles using nanosecond pulse laser ablation of titanium in liquid, gaseous and supercritical CO2. The produced particles were observed to be mainly anatase-TiO2 with some rutile-TiO2. In addition, the particles were covered by a carbon layer. Raman and X-ray diffraction data suggested that the rutile content increases with CO2 pressure. The nanoparticle size decreased and size distribution became narrower with the increase in CO2 pressure and temperature, however the variation trend was different for CO2 pressure compared to temperature. Pulsed laser ablation in pressurized CO2 is demonstrated as a single step method for making anatase-TiO2/carbon nanoparticles throughout the pressure and temperature ranges 5–40 MPa and 30–50 °C, respectively.
关键词： core-shell particles,pulsed laser ablation,nanoparticle size control,supercritical fluids
更新于2025-09-11 14:15:04