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1.
In this work a vapor-phase-assisted approach for the synthesis of monolayer MoS2 is demonstrated, based on the sulfurization of thin MoO3−x precursor films in an H2S atmosphere. We discuss the co-existence of various possible growth mechanisms, involving solid–gas and vapor–gas reactions. Different sequences were applied in order to control the growth mechanism and to obtain monolayer films. These variations include the sample temperature and a time delay for the injection of H2S into the reaction chamber. The optimized combination allows for tuning the process route towards the potentially more favorable vapor–gas reactions, leading to an improved material distribution on the substrate surface. Raman and photoluminescence (PL) spectroscopy confirm the formation of ultrathin MoS2 films on SiO2/Si substrates with a narrow thickness distribution in the monolayer range on length scales of a few millimeters. Best results are achieved in a temperature range of 950–1000 °C showing improved uniformity in terms of Raman and PL line shapes. The obtained films exhibit a PL yield similar to mechanically exfoliated monolayer flakes, demonstrating the high optical quality of the prepared layers.

Optimization of the sulfurization process of thin MoO3 precursor layers, pushing the reaction towards vapor-phase-assisted routes to obtain large-scale, homogeneous monolayer MoS2.  相似文献   

2.
Monolayer MoSe2 is a transition metal dichalcogenide with a narrow bandgap, high optical absorbance and large spin-splitting energy, giving it great promise for applications in the field of optoelectronics. Producing monolayer MoSe2 films in a reliable and scalable manner is still a challenging task as conventional chemical vapor deposition (CVD) or exfoliation based techniques are limited due to the small domains/nanosheet sizes obtained. Here, based on NaCl assisted CVD, we demonstrate the simple and stable synthesis of sub-millimeter size single-crystal MoSe2 monolayers with mobilities ranging from 38 to 8 cm2 V−1 s−1. The average mobility is 12 cm2 V−1 s−1. We further determine that the optical responsivity of monolayer MoSe2 is 42 mA W−1, with an external quantum efficiency of 8.22%.

Sub-millimeter single crystal MoSe2 monolayers with a mobility of 38 cm2 V−1 s−1 and responsivity of 42 mA W−1 were synthesized by NaCl-assisted chemical vapor deposition.  相似文献   

3.
4.
Constructing 2D inorganic perovskites and TMDs heterostructures is an effective method to design stable and high-performance perovskites optoelectronic applications. Here, we investigate the optoelectronic properties and interfacial interactions of Cs2PbX4–MSe2 (X = Cl, Br, I; M = Mo, W) heterostructures using first-principles calculations. Firstly, six Cs2PbX4–MSe2 interfaces remain stable in energy. With the halogen varying from Cl to I, the interlayer distances of Cs2PbX4–MSe2 heterostructures increase rapidly. The CBM and VBM of monolayer Cs2PbX4 are all higher than that of monolayer MSe2 and the charges transfer from Cs2PbX4 interfaces to MSe2 interfaces when they contact. Both Cs2PbX4–MSe2 heterostructures are type-II heterostructures, which can drive the photogenerated electrons and holes to move in opposite directions. What''s more, Cs2PbCl4–MoSe2 heterostructures exhibit the highest charge transport efficiency among Cs2PbX4–MoSe2 heterostructures because Cs2PbCl4–MoSe2 heterostructures have the lowest exciton binding energies among Cs2PbX4–MSe2 heterostructures. In addition, the optical absorptions of all heterostructures are significantly higher than the corresponding Cs2PbX4 monolayers and MSe2 monolayers. The construction of Cs2PbX4–MoSe2 heterostructures is beneficial for improving the photoelectric performance of two-dimensional perovskite devices. Lastly, we found that the Cs2PbI4–WSe2 heterostructure has the largest PCE (18%) among Cs2PbX4–MSe2 heterostructures. The Cs2PbCl4–MoSe2 heterostructure exhibits great potential application in photodetector devices and the Cs2PbI4–WSe2 heterostructure has great potential application in solar cells.

The PCE of Cs2PbX4–WSe2 heterostructures is larger than the PCE of Cs2PbX4–MoSe2 heterostructures. Cs2PbI4–WSe2 heterostructure has the largest PCE (18%) among Cs2PbX4–MSe2 heterostructures and has great potential application in solar cells.  相似文献   

5.
Here, we report the synthesis of a vertical MoSe2/WSe2 p–n heterostructure using a sputtering-CVD method. Unlike the conventional CVD method, this method produced a continuous MoSe2/WSe2 p–n heterostructure. WSe2 and MoSe2 back-gated field effect transistors (FETs) exhibited good gate modulation behavior, and high hole and electron mobilities of ∼2.2 and ∼15.1 cm2 V−1 s−1, respectively. The fabricated vertical MoSe2/WSe2 p–n diode showed rectifying IV behavior with back-gate tunability. The rectification ratio of the diode was increased with increasing gate voltage, and was increased from ∼18 to ∼1600 as the gate bias increased from −40 V to +40 V. This is attributed to the fact that the barrier height between p-WSe2 and n-MoSe2 is modulated due to the back-gate bias. The rectification ratio is higher than the previously reported values for the TMDC p–n heterostructure grown by CVD.

Here, we report a vertical MoSe2/WSe2 p–n heterostructure with rectifying IV behavior and back-gate tunability.  相似文献   

6.
Hybrid density functional has been adopted to investigate the structural, electronic, and optical properties of ZnO/MoS2 and ZnO/MoSe2 composites as compared with the results of ZnO, MoS2, and MoSe2 monolayers. The results indicate that MoS2 and MoSe2 monolayers could contact with monolayer ZnO to form ZnO/MoS2 and ZnO/MoSe2 heterostructures through van der Waals (vdW) interactions. The calculated bandgap of ZnO/MoS2 (ZnO/MoSe2) is narrower than that of ZnO or MoS2 (MoSe2) monolayers, facilitating the shift of light absorption edges of the composites towards visible light in comparison with bare ZnO and MoX2 monolayers. Through the application of strain, the ZnO/MoS2 and ZnO/MoSe2 composites which own suitable bandgaps, band edge positions, efficient charge separation, and good visible light absorption will be promising for visible light photocatalytic water splitting. These results provide a route for design and development of efficient ZnO/MoS2 and ZnO/MoSe2 photocatalysts for water splitting.

The ZnO/MoS2 (ZnO/MoSe2) heterostructures with the strain of –2% (+2%) have suitable bandgap and band edge position for hydrogen production via visible light photocatalytic water splitting.  相似文献   

7.
Fe3O4–Ag Janus composites were synthesized using a two-step solvothermal method. The optimal growth process was determined by investigating the relationship between the particle morphologies and reaction time. Magnetic and Raman spectroscopic measurements showed that the as-synthesized Janus composites have both good magnetic response and significant surface-enhanced Raman scattering (SERS) effects, as well as reproducibility. The calculated Raman enhancement factor reached an unprecedented magnitude of 109 compared with the values of other Fe3O4–Ag compounds. Furthermore, the SERS effect was exhibited even at a concentration of probe molecules as low as 10−13 M. This demonstrates that the as-synthesized Fe3O4–Ag Janus composite particles have promise for application as separable, highly sensitive SERS substrates.

Fe3O4–Ag Janus composites were synthesized using a two-step solvothermal method.  相似文献   

8.
The currently limited portfolio of volatile organoselenium compounds used for atomic layer deposition (ALD) has been extended by designing and preparing a series of four-, five- and six-membered cyclic silylselenides. Their fundamental properties were tailored by alternating the ring size, the number of embedded Se atoms and the used peripheral alkyl chains. In contrast to former preparations based on formation of sodium or lithium selenides, the newly developed synthetic method utilizes a direct and easy reaction of elemental selenium with chlorosilanes. Novel 2,2,4,4-tetraisopropyl-1,3,2,4-diselenadisiletane, which features good trade-off between chemical/thermal stability and reactivity, has been successfully used for gas-to-solid phase reaction with MoCl5 affording MoSe2. A thorough characterization of the as-deposited 2D MoSe2 flakes revealed its out-of-plane orientation and high purity. Hence, the developed four-membered cyclic silylselenide turned out to be well-suited Se-precursor for ALD of MoSe2.

Diselenadisiletanes possess easy preparation, tailored stability, reactivity, volatility and fast exchange ALD reaction to afford MoSe2 flakes of high quality.  相似文献   

9.
In the present study, we have developed a composite electrode of MSNT using a simple and scalable two-step scheme to synthesize a composite electrode material comprising MoSe2/multiwalled carbon nanotubes (MoSe2/MWCNTs) for supercapacitor applications. First, a MWCNT thin film was deposited on a stainless steel substrate by using a “dip and dry” coating technique. Subsequently, MoSe2 was deposited onto the MWCNT thin film using the successive ionic layer adsorption and reaction method. The lichen-like growth of MoSe2 on the MWCNT network provided dual charge storage and an effective ion transfer path. The composite electrode of MSNT has been studied systematically with different electrolytes and concentrations of electrolyte. As a result, the MoSe2/MWCNT (MSNT) electrode exhibited excellent electrochemical properties such as a specific capacity of 192 mA h g−1 and a capacitance retention of 88% after 2000 cycles in 1 M LiCl electrolyte. The results demonstrated the huge potential of the MSNT composite electrode for practical application in supercapacitors. The aqueous symmetric cell fabricated using the MSNT composite as both the anode and cathode showed an energy density of 17.9 W h kg−1. Additionally, the energy density improved by designing an asymmetric device of MSNT//MnO2 and notably, it reveals two-fold improvement in the energy density compared to a symmetric MSNT cell. The MSNT//MnO2-based asymmetric cell exhibited a maximum specific capacitance of 112 F g−1 with a high energy density of 35.6 W h kg−1.

Simple and scalable chemical synthesis approach to develop a MoSe2/MWCNTs composite thin film electrode for a highly efficient asymmetric supercapacitor cell.  相似文献   

10.
We investigated the homogeneity and tolerance to heat of monolayer MoS2 using photoluminescence (PL) spectroscopy. For MoS2 on SiO2, the PL spectra of the basal plane differ from those of the edge, but MoS2 on hexagonal boron nitride (h-BN) was electron-depleted with a homogeneous PL spectra over the entire area. Annealing at 450 °C rendered MoS2 on SiO2 homogeneously electron-depleted over the entire area by creating numerous defects; moreover, annealing at 550 °C and subsequent laser irradiation on the MoS2 monolayer caused a loss of its inherent crystal structure. On the other hand, monolayer MoS2 on h-BN was preserved up to 550 °C with its PL spectra not much changed compared with MoS2 on SiO2. We performed an experiment to qualitatively compare the binding energies between various layers, and discuss the tolerance of monolayer MoS2 to heat on the basis of interlayer/interfacial binding energy.

We investigated the homogeneity and tolerance to heat of monolayer MoS2 using photoluminescence (PL) spectroscopy.  相似文献   

11.
The high catalytic activity of cobalt-doped MoS2 (Co–MoS2) observed in several chemical reactions such as hydrogen evolution and hydrodesulfurization, among others, is mainly attributed to the formation of the CoMoS phase, in which Co occupies the edge-sites of MoS2. Unfortunately, its production represents a challenge due to limited cobalt incorporation and considerable segregation into sulfides and sulfates. We, therefore, developed a fast and efficient solid-state microwave irradiation synthesis process suitable for producing thin Co–MoS2 flakes (∼3–8 layers) attached on nitrogen-doped reduced graphene oxide. The CoMoS phase is predominant in samples with up to 15 at% of cobalt, and only a slight segregation into cobalt sulfides/sulfates is noticed at larger Co content. The Co–MoS2 flakes exhibit a large number of defects resulting in wavy sheets with significant variations in interlayer distance. The catalytic performance was investigated by evaluating the activity towards the hydrogen evolution reaction (HER), and a gradual improvement with increased amount of Co was observed, reaching a maximum at 15 at% with an overpotential of 197 mV at −10 mA cm−2, and a Tafel slope of 61 mV dec−1. The Co doping had little effect on the HER mechanism, but a reduced onset potential and charge transfer resistance contributed to the improved activity. Our results demonstrate the feasibility of using a rapid microwave irradiation process to produce highly doped Co–MoS2 with predominant CoMoS phase, excellent HER activity, and operational stability.

Production of nanostructured cobalt-doped MoS2 flakes with the CoMoS phase by microwave irradiation with improved catalytic activity towards hydrogen evolution.  相似文献   

12.
Molybdenum (Mo) is the most commonly used back-contact material for copper zinc tin selenide (CZTSe)-based thin-film solar cells. For most fabrication methods, an interfacial molybdenum diselenide (MoSe2) layer with an uncontrolled thickness is formed, ranging from a few tens of nm up to ≈1 μm. In order to improve the control of the back-contact interface in CZTSe solar cells, the formation of a MoSe2 layer with a homogeneous and defined thickness is necessary. In this study, we use plasma treatments on the as-grown Mo surface prior to the CZTSe absorber formation, which consists of the deposition of stacked metallic layers and the annealing in selenium (Se) atmosphere. The plasma treatments include the application of a pure argon (Ar) plasma and a mixed argon–nitrogen (Ar–N2) plasma. We observe a clear impact of the Ar plasma treatment on the MoSe2 thickness and interfacial morphology. With the Ar–N2 plasma treatment, a nitrided Mo surface can be obtained. Furthermore, we combine the Ar plasma treatment with the application of titanium nitride (TiN) as back-contact barrier and discuss the obtained results in terms of MoSe2 formation and solar cell performance, thus showing possible directions of back-contact engineering for CZTSe solar cells.

Molybdenum (Mo) is the most commonly used back-contact material for copper zinc tin selenide (CZTSe)-based thin-film solar cells. The effect of a pure Ar plasma and a mixed Ar–N2 plasma on the back-contact interface of CZTSe solar cells is reported in this study.  相似文献   

13.
The feasibility of laser cooling barium monohalides BaX (X = F, Cl, Br, I) is investigated using ab initio methods with the inclusion of spin–orbit coupling (SOC) effects. Calculated spectroscopic constants for BaF, BaCl, BaBr and BaI are in very good agreement with the available experimental measurements. The results demonstrate that the calculated electronic structure is accurate and can be used to establish the optical scheme of laser cooling. The highly diagonal Franck–Condon factors (FCFs) (BaF: f00 = 0.980, f11 = 0.939, f22 = 0.894; BaCl: f00 = 0.998, f11 = 0.995, f22 = 0.992) between the X2Σ+1/2 and A2Π1/2 states are determined, which are found to be in good agreement with previous theoretical results. The radiative lifetimes (BaF: 39.13–41.20 ns; BaCl: 117.99–110.23 ns) of the A2Π1/2–X2Σ+1/2 transition for the first five vibrational levels show that the A2Π1/2 is a rather short lifetime state. The current study indicates that BaF and BaCl are two good choices of molecules for laser cooling. Therefore, BaI and BaBr are not promising laser-cooling candidates because the FCFs of the A2Π1/2–X2Σ+1/2 transition are off-diagonal. We further propose the three-laser cooling schemes based on the A2Π1/2–X2Σ+1/2 transition for BaF and BaCl.

The feasibility of laser cooling barium monohalides BaX (X = F, Cl, Br, I) is investigated using ab initio methods with the inclusion of spin–orbit coupling (SOC) effects.  相似文献   

14.
In this study, two fluorescence conjugated microporous polymers based on perylene tetraanhydride bisimide (DP4A0 and DP4A2) were prepared via Sonogashira–Hagihara cross-coupling polymerization for the efficient detection of o-nitrophenol (o-NP). They were well characterized via FT-IR, solid state 13C NMR, elemental analysis, and other material characterization techniques. The experiments proved that both CMPs possess high thermal and chemical stability and a porous nature with Brunauer–Emmett–Teller (BET) specific surface areas of 41.3 and 402.1 m2 g−1. Importantly, owing to signal amplification by the conjugated skeleton, DP4A0 and DP4A2 exhibit extremely high sensitivity to o-NP with Ksv values of 1.83 × 104 and 1.69 × 104 L mol−1 and limits of detection of 5.73 × 10−9 and 7.36 × 10−9 mol L−1, respectively. The sensing performance of DP4A0 and DP4A2 was dependent on the position of crosslinking points and crosslinking density. Finally, super amplified quenching was considered the electron transfer mechanism and hydrogen bond interactions were also present.

In this study, two fluorescence conjugated microporous polymers based on perylene tetraanhydride bisimide (DP4A0 and DP4A2) were prepared via Sonogashira–Hagihara cross-coupling polymerization for the efficient detection of o-nitrophenol (o-NP).  相似文献   

15.
The weak light-absorption and low quantum yield (QY) in monolayer MoS2 are great challenges for the applications of this material in practical optoelectronic devices. Here, we report on a synergistic strategy to obtain highly enhanced photoluminescence (PL) of monolayer MoS2 by simultaneously improving the intensity of the electromagnetic field around MoS2 and the QY of MoS2. Self-assembled sub-monolayer Au nanoparticles underneath the monolayer MoS2 and bis(trifluoromethane)sulfonimide (TFSI) treatment to the MoS2 surface are used to boost the excitation field and the QY, respectively. An enhancement factor of the PL intensity as high as 280 is achieved. The enhancement mechanisms are analyzed by inspecting the contribution of the PL spectra from A excitons and A trions under different conditions. Our study takes a further step to developing high-performance optoelectronic devices based on monolayer MoS2.

A synergistic strategy is reported to obtain a highly enhanced photoluminescence (PL) of monolayer MoS2 by simultaneously improving the intensity of the electromagnetic field around MoS2 and the QY of MoS2.  相似文献   

16.
Monolithic polymer(resorcinol-formaldehyde) reinforced alumina (RF/Al2O3) aerogel composites were prepared using a sol–gel method and supercritical fluid CO2 drying. The formation mechanism, chemical compositions, pore structures, morphologies, thermal and mechanical performances of RF/Al2O3 aerogel composites with different RF/Al molar ratios were investigated. The results show that the two networks of organic resorcinol-formaldehyde and inorganic alumina are completely independent of one another. The as-synthesized RF/Al2O3 aerogels consist of spherical organic carbon particles and fibrous alumina, which possess low bulk density (0.077–0.112 g cm−3), low shrinkage (1.55–2.76%), low thermal conductivity (0.024–0.028 W m−1 K−1), and high specific surface area (453.26–722.75 m2 g−1). Especially, the sample prepared with molar ratio RF/Al = 1 shows the best network structure with the higher compressive strength (1.83 MPa) and Young''s modulus (122.57 MPa). The resulting robust RF/Al2O3 aerogel composites could be potentially used as thermal insulators, catalysts and adsorbents.

Monolithic polymer(resorcinol-formaldehyde) reinforced alumina (RF/Al2O3) aerogel composites were prepared using a sol–gel method and supercritical fluid CO2 drying.  相似文献   

17.
The depletion of fossil fuels and associated environmental problems have drawn our attention to renewable energy resources in order to meet the global energy demand. Electrocatalytic hydrogen evolution has been considered a potential energy solution due of its high energy density and environment friendly technology. Herein, we have successfully synthesized a noble-metal-free Co–Ni/MoS2 nanocomposite for enhanced electrocatalytic hydrogen evolution. The nanocomposite has been well characterized using HRTEM, elemental mapping, XRD, and XPS analysis. The as-synthesized nanocomposite exhibits a much smaller onset potential and better current density than those of Co–MoS2, Ni–MoS2 and MoS2, with a Tafel value of 49 mV dec−1, which is comparable to that of a commercial Pt/C catalyst. The synergistic effect and interfacial interaction of Co–Ni bimetallic nanoparticles enhances the intrinsic modulation in the electronic structure resulting in an improved HER performance. Moreover, the electrochemical impedance spectroscopic results suggest smaller resistance values for the Co–Ni/MoS2 nanocomposite, compared to those for the charge transfer of bare nanosheets, which increase the faradaic process and in turn enhance the HER kinetics for a better performance. Our as-synthesized Co–Ni/MoS2 nanocomposite holds great potential for the future synthesis of noble-metal-free catalysts.

A noble-metal-free Co–Ni/MoS2 nanocomposite was synthesized, which showed enhanced electrocatalytic hydrogen evolution performance.  相似文献   

18.
Two-dimensional (2D) heterojunctions with layered structures give high flexibility in varying their photocatalytic/electrocatalytic properties. Herein, 2D/2D heterostructures of MoS2/MoSe2 with different weight-ratios (1 : 1, 1 : 3, and 3 : 1) have been prepared by a simple one-step microwave-assisted technique. The characterization studies confirm formation of crystalline MoS2/MoSe2 nanoparticles with a high surface area (60 m2 g−1) and porous structure. The high synergistic-effect (1.73) and narrow bandgap (∼1.89 eV) of the composites result in enhanced photo-degradation efficiency towards methylene blue dye (94%) and fipronil pesticide (80%) with high rate constants (0.33 min−1 and 0.016 min−1 respectively) under visible light. The effect of pH, catalyst dose, and illumination area on photodegradation has been optimized. Photodegradation of real-industrial wastewater shows 65% COD and 51.5% TOC removal. Trapping experiments confirm that holes are mainly responsible for degradation. The composites were highly reusable showing 75% degradation after 5-cycles. MoS2/MoSe2 composites show excellent electrochemical water-splitting efficacy through hydrogen-evolution-reaction (HER) exhibiting a stable high current density of −19.4 mA cm−2 after 2500 cyclic-voltammetry (CV) cycles. The CV-plots reveal high capacitance activity (Cdl value ∼607 μF cm−2) with a great % capacitance retention (>90%). The as-prepared 2D/2D-catalysts are highly active in sunlight and beneficial for long-time physico-chemical wastewater treatment. Moreover, the electrochemical studies confirm that these composites are potential materials for HER activity and energy-storage applications.

The 2D/2D-MoS2/MoSe2 catalysts with good photocatalytic/electrocatalytic properties can be potential materials for wastewater treatment and hydrogen production.  相似文献   

19.
In this paper, CuO and CeO2 were screened as co-catalyst components for Fe2O3/attapulgite (ATP) catalyst, and three new catalysts (CuO–Fe2O3/ATP, CeO2–Fe2O3/ATP and CuO–CeO2–Fe2O3/ATP) were prepared for degradation of methylene blue (MB). The three catalysts'' characteristics were determined by BET, XRD, FT-IR, SEM and XPS. MB degradation in different systems and at different pH values was also studied. Under the conditions of H2O2 concentration of 4.9 mmol L−1, catalyst dosage of 5 g L−1, pH of 5, reaction temperature of 60 °C and MB initial concentration of 100 mg L−1, the as-synthesized catalysts showed much greater reaction rate and degradation efficiency of MB than Fe2O3/ATP catalyst. In addition, the reusability of the as-prepared composites was evaluated. The intermediate products of MB degradation were identified by LC-MS and the possible degradation process of MB was put forward.

A novel heterogeneous catalyst CuO–CeO2–Fe2O3/ATP was synthesized for MB degradation and the catalytic mechanism was put forward.  相似文献   

20.
Correction for ‘A vertical WSe2–MoSe2 p–n heterostructure with tunable gate rectification’ by Hailing Liu et al., RSC Adv., 2018, 8, 25514–25518.

The authors regret that Hailiang Liu’s name was spelled incorrectly in the original article; the corrected version is shown above.The Royal Society of Chemistry apologises for these errors and any consequent inconvenience to authors and readers.  相似文献   

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