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1.
Two‐dimensional (2D) nanomaterials and heterostructured nanocrystals (NCs) are two hot topics in current nanoresearch. However, reports on heterostructured NCs with 2D features are still rare. In this work, we demonstrate a one‐pot colloidal chemistry route for synthesizing Au‐CuZnSe2 heterostructures with spherical Au domains attached to the edge of a sheet of CuZnSe2. This protocol involves the preferential formation of Au clusters and the seeded growth of CuZnSe2 sheets because of the lattice matching of CuSe with Au. As an example to demonstrate the importance of such heterostructures, the electrochemical performance of Au‐CuZnSe2 heterostructured nanosheets is compared with that of heterostructured nanorods, Au NCs, and CuZnSe2 NCs. The heterostructured nanosheets exhibit the best electrochemical activity.  相似文献   

2.
All‐inorganic perovskites have high carrier mobility, long carrier diffusion length, excellent visible light absorption, and well overlapping with localized surface plasmon resonance (LSPR) of noble metal nanocrystals (NCs). The high‐performance photodetectors can be constructed by means of the intrinsic outstanding photoelectric properties, especially plasma coupling. Here, for the first time, inorganic perovskite photodetectors are demonstrated with synergetic effect of preferred‐orientation film and plasmonic with both high performance and solution process virtues, evidenced by 238% plasmonic enhancement factor and 106 on/off ratio. The CsPbBr3 and Au NC inks are assembled into high‐quality films by centrifugal‐casting and spin‐coating, respectively, which lead to the low cost and solution‐processed photodetectors. The remarkable near‐field enhancement effect induced by the coupling between Au LSPR and CsPbBr3 photogenerated carriers is revealed by finite‐difference time‐domain simulations. The photodetector exhibits a light on/off ratio of more than 106 under 532 nm laser illumination of 4.65 mW cm?2. The photocurrent increases from 0.67 to 2.77 μA with centrifugal‐casting. Moreover, the photocurrent rises from 245.6 to 831.1 μA with Au NCs plasma enhancement, leading to an enhancement factor of 238%, which is the most optimal report among the LSPR‐enhanced photodetectors, to the best of our knowledge. The results of this study suggest that all‐inorganic perovskites are promising semiconductors for high‐performance solution‐processed photodetectors, which can be further enhanced by Au plasmonic effect, and hence have huge potentials in optical communication, safety monitoring, and biological sensing.  相似文献   

3.
2D Molybdenum disulfide (MoS2) is a promising candidate material for high‐speed and flexible optoelectronic devices, but only with low photoresponsivity. Here, a large enhancement of photocurrent response is obtained by coupling few‐layer MoS2 with Au plasmonic nanostructure arrays. Au nanoparticles or nanoplates placed onto few‐layer MoS2 surface can enhance the local optical field in the MoS2 layer, due to the localized surface plasmon (LSP) resonance. After depositing 4 nm thick Au nanoparticles sparsely onto few‐layer MoS2 phototransistors, a doubled increase in the photocurrent response is observed. The photocurrent of few‐layer MoS2 phototransistors exhibits a threefold enhancement with periodic Au nanoarrays. The simulated optical field distribution confirms that light can be trapped and enhanced near the Au nanoplates. These findings offer an avenue for practical applications of high performance MoS2‐based optoelectronic devices or systems in the future.  相似文献   

4.
2D materials hold great potential for designing novel electronic and optoelectronic devices. However, 2D material can only absorb limited incident light. As a representative 2D semiconductor, monolayer MoS2 can only absorb up to 10% of the incident light in the visible, which is not sufficient to achieve a high optical‐to‐electrical conversion efficiency. To overcome this shortcoming, a “gap‐mode” plasmon‐enhanced monolayer MoS2 fluorescent emitter and photodetector is designed by squeezing the light‐field into Ag shell‐isolated nanoparticles–Au film gap, where the confined electromagnetic field can interact with monolayer MoS2. With this gap‐mode plasmon‐enhanced configuration, a 110‐fold enhancement of photoluminescence intensity is achieved, exceeding values reached by other plasmon‐enhanced MoS2 fluorescent emitters. In addition, a gap‐mode plasmon‐enhanced monolayer MoS2 photodetector with an 880% enhancement in photocurrent and a responsivity of 287.5 A W?1 is demonstrated, exceeding previously reported plasmon‐enhanced monolayer MoS2 photodetectors.  相似文献   

5.
A generalized scheme for the fabrication of high performance photodetectors consisting of a p‐type channel material and n‐type nanoparticles is proposed. The high performance of the proposed hybrid photodetector is achieved through enhanced photoabsorption and the photocurrent gain arising from its effective charge transfer mechanism. In this paper, the realization of this design is presented in a hybrid photodetector consisting of 2D p‐type black phosphorus (BP) and n‐type molybdenum disulfide nanoparticles (MoS2 NPs), and it is demonstrated that it exhibits enhanced photoresponsivity and detectivity compared to pristine BP photodetectors. It is found that the performance of hybrid photodetector depends on the density of NPs on BP layer and that the response time can be reduced with increasing density of MoS2 NPs. The rising and falling times of this photodetector are smaller than those of BP photodetectors without NPs. This proposed scheme is expected to work equally well for a photodetector with an n‐type channel material and p‐type nanoparticles.  相似文献   

6.
The unique properties of MoS2 nanosheets make them a promising candidate for high‐performance room temperature sensing. However, the properties of pristine MoS2 nanosheets are strongly influenced by the significant adsorption of oxygen in an air environment, which leads to instability of the MoS2 sensing device, and all sensing results on MoS2 reported to date were exclusively obtained in an inert atmosphere. This significantly limits the practical sensor application of MoS2 in an air environment. Herein, a novel nanohybrid of SnO2 nanocrystal (NC)‐decorated crumpled MoS2 nanosheet (MoS2/SnO2) and its exciting air‐stable property for room temperature sensing of NO2 are reported. Interestingly, the SnO2 NCs serve as strong p‐type dopants for MoS2, leading to p‐type channels in the MoS2 nanosheets. The SnO2 NCs also significantly enhance the stability of MoS2 nanosheets in dry air. As a result, unlike other MoS2 sensors operated in an inert gas (e.g. N2), the nanohybrids exhibit high sensitivity, excellent selectivity, and repeatability to NO2 under a practical dry air environment. This work suggests that NC decoration significantly tunes the properties of MoS2 nanosheets for various applications.  相似文献   

7.
Hydrogen production from water splitting through an efficient photoelectrochemical route requires photoinduced electron transfer from light harvesters to efficient electrocatalysts. Here, the plasmon‐enhanced photoelectrical nanocatalysts (NCs) have been successfully developed by coating a monolayer MoS2 on the Cu1.75S‐Au hetero‐nanoparticle for hydrogen evolution reaction (HER). The plasmonic NCs dramatically improve the HER, leading to 29.5‐fold increase of current under 650 nm excitation (1.0 W cm?2). These NCs generate an exceptionally high current density of 200 mA cm?2 at overpotential of 182.8 mV with a Tafel slope of 39 mV per decade and excellent stability, which is better than or comparable to the Pt‐free catalysts with carbon rod as counter electrode. The enhanced HER performance can be attributed to the significantly improved broad light absorption (400–3000 nm), more efficient charge separation and abundant active edge sites of monolayer MoS2. The studies may provide a facile strategy for the fabrication of efficient plasmon‐enhanced photoelectrical NCs for HER.  相似文献   

8.
The exploitation of nanoconfined conversion of Au‐ and Pt‐containing binary nanocrystals for developing a controllable synthesis of surfactant‐free AuPt nanocrystals with enhanced formic acid oxidation (FAO) activity is reported, which can be stably and evenly immobilized on various support materials to diversify and optimize their electrocatalytic performance. In this study, an atomic layer of Pt2+ species is discovered to be spontaneously deposited in situ on the Au nanocrystal generated from a reverse‐microemulsion solution. The resulting Au/Pt2+ nanocrystal thermally transforms into a reduced AuPt alloy nanocrystal during the subsequent solid‐state conversion process within the SiO2 nanosphere. The alloy nanocrystals can be isolated from SiO2 in a surfactant‐free form and then dispersedly loaded on the carbon sphere surface, allowing for the production of a supported electrocatalyst that exhibits much higher FAO activity than commercial Pt/C catalysts. Furthermore, by involving Fe3O4 nanocrystals in the conversion process, the AuPt alloy nanocrystals can be grown on the oxide surface, improving the durability of supported metal catalysts, and then uniformly loaded on a reduced graphene oxide (RGO) layer with high electroconductivity. This produces electrocatalytic AuPt/Fe3O4/RGO nanocomposites whose catalyst‐oxide‐graphene triple‐junction structure provides improved electrocatalytic properties in terms of both activity and durability in catalyzing FAO.  相似文献   

9.
Controllable and efficient synthesis of noble metal/transition‐metal oxide (TMO) composites with tailored nanostructures and precise components is essential for their application. Herein, a general mercaptosilane‐assisted one‐pot coassembly approach is developed to synthesize ordered mesoporous TMOs with agglomerated‐free noble metal nanoparticles, including Au/WO3, Au/TiO2, Au/NbOx, and Pt/WO3. 3‐mercaptopropyl trimethoxysilane is applied as a bridge agent to cohydrolyze with metal oxide precursors by alkoxysilane moieties and interact with the noble metal source (e.g., HAuCl4 and H2PtCl4) by mercapto (? SH) groups, resulting in coassembly with poly(ethylene oxide)‐b‐polystyrene. The noble metal decorated TMO materials exhibit highly ordered mesoporous structure, large pore size (≈14–20 nm), high specific surface area (61–138 m2 g?1), and highly dispersed noble metal (e.g., Au and Pt) nanoparticles. In the system of Au/WO3, in situ generated SiO2 incorporation not only enhances their thermal stability but also induces the formation of ε‐phase WO3 promoting gas sensing performance. Owning to its specific compositions and structure, the gas sensor based on Au/WO3 materials possess enhanced ethanol sensing performance with a good response (Rair/Rgas = 36–50 ppm of ethanol), high selectivity, and excellent low‐concentration detection capability (down to 50 ppb) at low working temperature (200 °C).  相似文献   

10.
Galvanic replacement reactions (GRRs) on nanoparticles (NPs) are typically performed between two metals, i.e., a solid metal NP and a replacing salt solution of a more noble metal. The solution pH in GRRs is commonly considered an irrelevant parameter. Yet, the solution pH plays a major role in GRRs involving metal oxide NPs. Here, Cu2O nanocrystals (NCs) are studied as galvanic replacement (GR) precursors, undergoing replacement by gold and palladium, with the resulting nanostructures showing a strong dependence on the pH of the replacing metal salt solution. GRRs are reported for the first time on supported (chemically deposited) oxide NCs and the results are compared with those obtained with corresponding colloidal systems. Control of the pH enables production of different nanostructures, from metal‐decorated Cu2O NCs to uniformly coated Cu2O‐in‐metal (Cu2O@Me) core–shell nanoarchitectures. Improved metal nucleation efficiencies at low pHs are attributed to changes in the Cu2O surface charge resulting from protonation of the oxide surface. GR followed by etching of the Cu2O cores provides metal nanocages that collapse upon drying; the latter is prevented using a sol–gel silica overlayer stabilizing the metal nanocages. Metal‐replaced Cu2O NCs and their corresponding stabilized nanostructures may be useful as photocatalysts, electrocatalysts, and nanosensors.  相似文献   

11.
2D transition metal carbides, known as MXenes, are transparent when the samples are thin enough. They are also excellent electrical conductors with metal‐like carrier concentrations. Herein, these characteristics are exploited to replace gold (Au) in GaAs photodetectors. By simply spin‐coating transparent Ti3C2‐based MXene electrodes from aqueous suspensions onto GaAs patterned with a photoresist and lifted off with acetone, photodetectors that outperform more standard Au electrodes are fabricated. Both the Au‐ and MXene‐based devices show rectifying contacts with comparable Schottky barrier heights and internal electric fields. The latter, however, exhibit significantly higher responsivities and quantum efficiencies, with similar dark currents, hence showing better dynamic range and detectivity, and similar sub‐nanosecond response speeds compared to the Au‐based devices. The simple fabrication process is readily integratable into microelectronic, photonic‐integrated circuits and silicon photonics processes, with a wide range of applications from optical sensing to light detection and ranging and telecommunications.  相似文献   

12.
Molybdenum disulfide (MoS2), a typical 2D metal dichalcogenide (2DMD), has exhibited tremendous potential in optoelectronic device applications, especially in photodetection. However, due to the weak light absorption of planar mono‐/multilayers, limited cutoff wavelength edge, and lack of high‐quality junctions, most reported MoS2‐based photodetectors show undesirable performance. Here, a structurized 3D heterojunction of RGO–MoS2/pyramid Si is demonstrated via a simple solution‐processing method. Owing to the improved light absorption by the pyramid structure, the narrowed bandgap of the MoS2 by the imperfect crystallinity, and the enhanced charge separation/transportation by the inserted reduced graphene oxide (RGO), the assembled photodetector exhibits excellent performance in terms of a large responsivity of 21.8 A W?1, extremely high detectivity up to 3.8 × 1015 Jones (Jones = cm Hz1/2 W?1) and ultrabroad spectrum response ranging from 350 nm (ultraviolet) to 4.3 µm (midwave infrared). These device parameters represent the best results for MoS2‐based self‐driven photodetectors, and the detectivity value sets a new record for the 2DMD‐based photodetectors reported thus far. Prospectively, the design of novel 3D heterojunction can be extended to other 2DMDs, opening up the opportunities for a host of high‐performance optoelectronic devices.  相似文献   

13.
The surface structure‐controlled synthesis of noble metal nanocrystals (NCs) bounded by high‐index facets has become a hot research topic due to their potential to significantly improve catalytic performance. This study reports the preparation of monodisperse Au–Pd alloy NCs with systematic shape evolution from rhombic dodecahedral (RD) to trisoctahedral (TOH), and hexoctahedral (HOH) structures by varying the concentration of surfactant in the surfactant‐mediated synthesis. The as‐prepared three kinds of alloy NCs possess almost the same size and composition as each other. It is suggested that the surfactant containing long‐chain octadecyltrimethyl ammonium (OTA+) ions plays a key role in the formation of high index facets, and the crystal growth kinetics may also have an effect on the formation of different nanocrystal morphologies. In addition, the catalytic activities of these NCs are evaluated by structure‐sensitive reactions, including ethanol electro‐oxidation and the catalytic reduction of 4‐nitrophenol (4‐NPh). These three types of Au–Pd alloy NCs exhibit different catalytic selectivities towards these two reactions. The catalytic activities toward electro‐oxidation of ethanol are in the order of HOH > RD > TOH, which follows the order of their corresponding surface energies. However, the activities toward catalytic reduction of 4‐NPh are in the order of RD > TOH > HOH, which should be related to the local structure of the surfaces.  相似文献   

14.
Recycling of noble metal from waste materials, namely from electronic wastes (e‐waste), spent catalyst, and industrial wastewater, is attracting growing attention due to the scarcity, economic importance, and criticality of those noble metals. Traditional techniques reported to date require toxic reagent and strict extraction conditions, which deeply hinders the development of precious metal recovery in complex environments. Here, an approach is proposed that uses flexible metallic transition metal dichalcogenide (TMD) paper, which provides abundant active sites for spontaneous adsorption and reduction of noble metal ions, as an Alchemy‐inspired template to recover noble metal in an efficient and green way without the aid of reductant and heating. The metallic TMD (MoS2, WS2) paper is shown to rapidly extract five noble metal ions (Au, Pd, Pt, Ag, and Ru) from complex samples containing various interferents. This unique property endows the metallic TMD paper with gifted ability in extracting gold from e‐waste, and recovering platinum group metals (palladium and platinum) from spent catalysts, which provides a blueprint for the design of next‐generation green platforms for noble metal regeneration.  相似文献   

15.
2D molybdenum disulfide (MoS2) possesses excellent optoelectronic properties that make it a promising candidate for use in high‐performance photodetectors. Yet, to meet the growing demand for practical and reliable MoS2 photodetectors, the critical issue of defect introduction to the interface between the exfoliated MoS2 and the electrode metal during fabrication must be addressed, because defects deteriorate the device performance. To achieve this objective, the use of an atomic layer‐deposited TiO2 interlayer (between exfoliated MoS2 and electrode) is reported in this work, for the first time, to enhance the performance of MoS2 photodetectors. The TiO2 interlayer is inserted through 20 atomic layer deposition cycles before depositing the electrode metal on MoS2/SiO2 substrate, leading to significantly enhanced photoresponsivity and response speed. These results pave the way for practical applications and provide a novel direction for optimizing the interlayer material.  相似文献   

16.
MoS2 quantum dots (QDs)‐based white‐light‐emitting diodes (QD‐WLEDs) are designed, fabricated, and demonstrated. The highly luminescent, histidine‐doped MoS2 QDs synthesized by microwave induced fragmentation of 2D MoS2 nanoflakes possess a wide distribution of available electronic states as inferred from the pronounced excitation‐wavelength‐dependent emission properties. Notably, the histidine‐doped MoS2 QDs show a very strong emission intensity, which exceeds seven times of magnitude larger than that of pristine MoS2 QDs. The strongly enhanced emission is mainly attributed to nitrogen acceptor bound excitons and passivation of defects by histidine‐doping, which can enhance the radiative recombination drastically. The enabled electroluminescence (EL) spectra of the QD‐WLEDs with the main peak around 500 nm are found to be consistent with the photoluminescence spectra of the histidine‐doped MoS2 QDs. The enhanced intensity of EL spectra with the current increase shows the stability of histidine‐doped MoS2 based QD‐WLEDs. The typical EL spectrum of the novel QD‐WLEDs has a Commission Internationale de l'Eclairage chromaticity coordinate of (0.30, 0.36) exhibiting an intrinsic broadband white‐light emission. The unprecedented and low‐toxicity QD‐WLEDs based on a single light‐emitting material can serve as an excellent alternative for using transition metal dichalcogenides QDs as next generation optoelectronic devices.  相似文献   

17.
Surface modification or decoration of ultrathin MoS2 films with chemical moieties is appealing since nanointerfacing can functionalize MoS2 films with bonus potentials. In this work, a facile and effective method for microlandscaping of Au nanoparticles (NPs) on few‐layer MoS2 films is developed. This approach first employs a focused laser beam to premodify the MoS2 films to achieve active surface domains with unbound sulfur. When the activated surface is subsequently immersed in AuCl3 solution, Au NPs are found to preferentially decorate onto the modified regions. As a result, Au NPs can be selectively and locally anchored onto designated regions on the MoS2 surface. With a scanning laser beam, microlandscapes comprising of Au NPs decorated on laser‐defined micropatterns are constructed. By varying the laser power, reaction time and thickness of the MoS2 films, the size and density of the NPs can be controlled. The resulting hybrid materials are demonstrated as efficient Raman active surfaces for the detection of aromatic molecules with high sensitivity.  相似文献   

18.
Developing earth‐abundant and efficient electrocatalysts for photoelectrochemical water splitting is critical to realizing a high‐performance solar‐to‐hydrogen energy conversion process. Herein, phosphorus‐rich colloidal cobalt diphosphide nanocrystals (CoP2 NCs) are synthesized via hot injection. The CoP2 NCs show a Pt‐like hydrogen evolution reaction (HER) electrocatalytic activity in acidic solution with a small overpotential of 39 mV to achieve ?10 mA cm?2 and a very low Tafel slope of 32 mV dec?1. Density functional theory (DFT) calculations reveal that the high P content both physically separates Co atoms to prevent H from over binding to multiple Co atoms, while simultaneously stabilizing H adsorbed to single Co atoms. The catalytic performance of the CoP2 NCs is further demonstrated in a metal–insulator–semiconductor photoelectrochemical device consisting of bottom p‐Si light absorber, atomic layer deposition Al–ZnO passivation layers, and the CoP2 cocatalyst. The p‐Si/AZO/TiO2/CoP2 photocathode shows a photocurrent density of ?16.7 mA cm?2 at 0 V versus reversible hydrogen electrode (RHE) and an output photovoltage of 0.54 V. The high performance and stability are attributed to the junction between p‐Si and AZO, the corrosion‐resistance of the pinhole‐free TiO2 protective layer, and the fast HER kinetics of the CoP2 NCs.  相似文献   

19.
2D transition metal dichalcogenides have attracted much attention in the field of spintronics due to their rich spin‐dependent properties. The promise of highly compact and low‐energy‐consumption spin‐orbit torque (SOT) devices motivates the search for structures and materials that can satisfy the requirements of giant perpendicular magnetic anisotropy (PMA) and large SOT simultaneously in SOT‐based magnetic memory. Here, it is demonstrated that PMA and SOT in a heavy metal/transition metal ferromagnet structure, Pt/[Co/Ni]2, can be greatly enhanced by introducing a molybdenum disulfide (MoS2) underlayer. According to first‐principles calculation and X‐ray absorption spectroscopy (XAS), the enhancement of the PMA is ascribed to the modification of the orbital hybridization at the interface of Pt/Co due to MoS2. The enhancement of SOT by the role played by MoS2 is explained, which is strongly supported by the identical behavior of SOT and PMA as a function of Pt thickness. This work provides new possibilities to integrate 2D materials into promising spintronics devices.  相似文献   

20.
Currently 2D crystals are being studied intensively for use in future nanoelectronics, as conventional semiconductor devices face challenges in high power consumption and short channel effects when scaled to the quantum limit. Toward this end, achieving barrier‐free contact to 2D semiconductors has emerged as a major roadblock. In conventional contacts to bulk metals, the 2D semiconductor Fermi levels become pinned inside the bandgap, deviating from the ideal Schottky–Mott rule and resulting in significant suppression of carrier transport in the device. Here, MoS2 polarity control is realized without extrinsic doping by employing a 1D elemental metal contact scheme. The use of high‐work‐function palladium (Pd) or gold (Au) enables a high‐quality p‐type dominant contact to intrinsic MoS2, realizing Fermi level depinning. Field‐effect transistors (FETs) with Pd edge contact and Au edge contact show high performance with the highest hole mobility reaching 330 and 432 cm2 V?1 s?1 at 300 K, respectively. The ideal Fermi level alignment allows creation of p‐ and n‐type FETs on the same intrinsic MoS2 flake using Pd and low‐work‐function molybdenum (Mo) contacts, respectively. This device acts as an efficient inverter, a basic building block for semiconductor integrated circuits, with gain reaching 15 at VD = 5 V.  相似文献   

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