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1.
PbSe semiconductor nanocrystals (NCs) have attracted ever‐growing interest owing to both their fundamental physics and potential applications in a diverse range of fields such as optoelectronic devices and nonlinear optics. The current fabrication strategy for colloidal PbSe NCs, however, frequently involves acutely toxic reagents and tedious reaction procedures, and is plagued by products with poorly controlled size and morphology. Herein, we report a facile, low‐cost, and phosphine‐free method for synthesizing PbSe NCs, which provides highly uniform NCs with tunable mid‐IR absorption, and they are promising for bio‐related applications. These high quality NCs were obtained by the reaction of elemental Se and PbCl2 in oleylamine as both the ligand and reaction medium. The high flexibility and reproducibility of the method reported in this study allows us to synthesize monodispersed PbSe NCs with well‐controlled size and morphology. In addition, these products show strong optical limiting effects, and thus hold potential for developing nonlinear optical devices.  相似文献   

2.
Capping ligands are indispensable for the preparation of metal-halide-perovskite (MHP) nanocrystals (NCs) with good stability; however, the long alkyl-chain capping ligands in conventional MHP NCs will be unfavorable for CO2 adsorption and hinder the efficient carrier separation on the surface of MHP NCs, leading to inferior catalytic activity in artificial photosynthesis. Herein, CsPbBr3 nanocrystals with short-chain glycine as ligand are constructed through a facile ligand-exchange strategy. Owing to the reduced hindrance of glycine and the presence of the amine group in glycine, the photogenerated carrier separation and CO2 uptake capacity are noticeably improved without compromising the stability of the MHP NCs. The CsPbBr3 nanocrystals with glycine ligands exhibit a significantly increased yield of 27.7 μmol g−1 h−1 for photocatalytic CO2-to-CO conversion without any organic sacrificial reagents, which is over five times higher than that of control CsPbBr3 NCs with conventional long alkyl-chain capping ligands.  相似文献   

3.
Colloid nanocrystals (NCs) mainly include metal nanocrystals, semiconductor nanocrystals, and insulator nanocrystals, exhibiting interesting size-dependent electrical, optical, magnetic, and chemical properties that cannot be achieved by their bulk counterparts. However, there’s a critical problem that NCs tend to aggregate, which induces degradation of their performance. Hyperbranched polymers (HPs) possess excellent attributes of three-dimensional topology, low viscosity, good solubility, and plenty of modifiable terminal groups. The combination of NCs and HPs to form nanohybrids cannot only endow NCs with multifunctionality, uniform dispersibility, and splendid solubility but also can impart extra properties to HPs. This article reviews the recent progress and state-of-the-art of the synthesis and applications of NCs-HPs nanohybrids (NHBs). NHBs can be obtained by three approaches: HPs first (i.e., NCs are formed with the stabilizer of HPs), NCs first (i.e., HPs are grafted on the surface of as-prepared NCs), and ligand exchange (the original ligand of NCs is replaced with HPs). Various HPs including hyperbranched poly(amidoamine), polyethylenimine, polyglycerol, polyester, polyamide, polyurethane, and poly(3-ethyl-3-hydroxymethyloxetane), as well as sorts of NCs such as metals (e.g., Ag, Au, Pd, Pt, and Rh), quantum dots (e.g., ZnO, CdS, CdTe, CdSe, and SnO2), magnetic oxides (e.g., Fe3O4), rare earth compounds, and so forth, have been used to obtain NHBs. The NHBs can be applied in nanocatalysis, antimicrobia, biosensor, biological labeling, and other fields promising their bright future.  相似文献   

4.
In the present work, CdSe nanocrystals (NCs) synthesized with a trioctylphosphine surface passivation layer were modified using amphiphilic molecules to form a surface bilayer capable of providing stable NCs aqueous solutions. Such modified nanocrystals were used as a test solute in order to analyze new electrophoretic phenomena, by applying a micellar plug as a separation tool for discriminating nanocrystals between micellar and micelle-free zones during electrophoresis. The distribution of NCs between both zones depended on the affinity of nanocrystals towards the micellar zone, and this relies on the kind of surface ligands attached to the NCs, as well as electrophoretic conditions applied. In this case, the NCs that migrated within a micellar zone can be focused using a preconcentration mechanism. By modifying electrophoretic conditions, NCs were forced to migrate outside the micellar zone in the form of a typical CZE peak. In this situation, a two-order difference in separation efficiencies, in terms of theoretical plates, was observed between focused NCs (N ~ 107) and a typical CZE peak for NCs (N ~ 105). By applying the amino-functionalized NCs the preconcentration of NCs, using a micellar plug, was examined, with the conclusion that preconcentration efficiency, in terms of the enhancement factor for peak height (SEFheight) can be, at least 20. The distribution effect was applied to separate CdSe/ZnS NCs encapsulated in silica, as well as surface-modified with DNA, which allows the estimation of the yield of conjugation of biologically active molecules to a particle surface.  相似文献   

5.
Cesium lead halide (CsPbX3: X = I, Br, Cl) nanocrystals (NCs) are believed to be potential candidates for bioimaging applications. However, their low structural stability against polar solvents remains as a major limitation. To improve the NCs stability and maintain high emission intensity, we synthesized silica coated Zn-doped core@shell perovskite NCs via modified ligand assisted reprecipitation (LARP) synthetic method under relatively high humid condition. We systemically varied the composition inside the perovskite structure and then studied their photophysical properties and stability. Interestingly, the Zn-doping amount controls the ratio of CsPbBr3 to Cs4PbBr6 perovskites inside the core and also facilitates the growth of (OA)2PbBr4 shell, enables overall increase in NCs emission intensity and stability. We observed green color emission from these NCs in the spectral range of 494-506 nm with a maximum photoluminescence quantum yield (PLQY) up to 88%. The optimized Zn-doped NCs exhibited nearly four times better water stability compared to the bare NCs and retain emission properties for several months even in highly polar solvents. Finally, we performed biocompatibility test of the NCs generated on biological samples and hydroponics test in a gardenia leaf for their potential bioimaging applications.  相似文献   

6.
SnFe2O4 nanocrystals (NC), prepared with a simple one‐step carrier‐solvent‐assisted interfacial reaction process, were developed as highly efficient catalysts for hydrogen peroxide sensing. These NCs, with a size of around 7 nm, served as the sensing catalyst and were decorated onto the pore surfaces of a porous fluorine‐doped tin oxide (PFTO) host electrode, prepared from commercial FTO glass with a simple anodic treatment, to form the sensing electrode for hydrogen peroxide. The SnFe2O4 NCs‐loaded PFTO electrode exhibited an ultra‐high sensitivity of 1027 mA m ?1 cm?2 toward hydrogen peroxide, outperforming Pt NCs‐loaded PFTO electrodes. The SnFe2O4 NCs‐loaded PFTO electrode proved a promising relatively low cost, high performance sensing electrode for hydrogen peroxide.  相似文献   

7.
We describe the simple, scalable, single‐step, and polar‐solvent‐free synthesis of high‐quality colloidal CsPbX3 (X=Cl, Br, and I) perovskite nanocrystals (NCs) with tunable halide ion composition and thickness by direct ultrasonication of the corresponding precursor solutions in the presence of organic capping molecules. High angle annular dark field scanning transmission electron microscopy (HAADF‐STEM) revealed the cubic crystal structure and surface termination of the NCs with atomic resolution. The NCs exhibit high photoluminescence quantum yields, narrow emission line widths, and considerable air stability. Furthermore, we investigated the quantum size effects in CsPbBr3 and CsPbI3 nanoplatelets by tuning their thickness down to only three to six monolayers. The high quality of the prepared NCs (CsPbBr3) was confirmed by amplified spontaneous emission with low thresholds. The versatility of this synthesis approach was demonstrated by synthesizing different perovskite NCs.  相似文献   

8.
Exploiting high‐performance and inexpensive electrocatalysts for methanol electro‐oxidation is conductive to promoting the commercial application of direct methanol fuel cells. Here, we present a facile synthesis of echinus‐like PdCu nanocrystals (NCs) via a one‐step and template‐free method. The echinus‐like PdCu NCs possess numerous straight and long branches which can provide abundant catalytic active sites. Owing to the novel nanoarchitecture and electronic effect of the PdCu alloy, the echinus‐like PdCu NCs display high electrocatalytic performance toward methanol oxidation reaction in an alkaline medium. The mass activity of echinus‐like PdCu NCs is 1202.1 mA mgPd?1, which is 3.7 times that of Pd/C catalysts. In addition, the echinus‐like structure, as a kind of three‐dimensional self‐supported nanoarchitecture, endows PdCu NCs with significantly enhanced stability and durability. Hence, the echinus‐like PdCu NCs hold prospect of being employed as electrocatalysts for direct alcohol fuel cells.  相似文献   

9.
Nitrogen-doped TiO2 nanocrystals (N−TiO2 NCs) were simply synthesized and then functionalized with streptavidin for highly sensitive electrochemical immunoassay of tumor marker. Scanning electron microscopy, transmission electron microscopy, static water contact angle, and cyclic voltametric measurement were adapted to examine the properties of N−TiO2 NCs and resultant immunosensor. The functionalized N−TiO2 NCs sensing platform shows high electrochemical conductivity, large surface area and excellent hydrophilicity. The features make them to produce high current response, capture more antibody molecules, and maintain the bioactivity of immobilized antibodies. By means of carcinoembryonic antigen (CEA) as model tumor marker, a wide linear range of 0.005–3 ng/mL and a low detection limit of 0.005 ng/mL (signal-to-noise ratio of 3) were achieved by the proposed CEA immunosensor. Furthermore, the resultant CEA immunosensor displays high specificity and was employed to determine CEA in clinical serum samples.  相似文献   

10.
Zhouping Wang  Jun Li  Jinghong Li 《Talanta》2009,77(3):1050-319
It was found that the mixing of CdTe semiconductor nanocrystals (NCs) with luminol in the presence of KMnO4 can induce a great sensitized effect on chemiluminescence (CL) emission. When the concentration of luminol, KMnO4 and NaOH were fixed at 1 μM, 1 μM and 0.05 M, respectively, the most excellent performance can be obtained for the CdTe NCs sensitized CL. By means of CL and photoluminescence spectra, we suppose the enhanced CL signals resulted from the accelerated luminol CL induced by the oxidized species of CdTe NCs. Based on the finding, using thioglycolic acid-capped CdTe NCs as label and immunoglobulin G (IgG) as a model analyte, a CL immunoassay protocol for IgG content detection was developed. The strong inhibition effect of phenol compounds on luminol-KMnO4-CdTe NCs CL system was also observed. All these findings demonstrated the possibility of semiconductor nanocrystals induced chemiluminescence to be utilized for more practical applications.  相似文献   

11.
The kinetics of borane transfer from simple tertiary phosphine borane adducts to a wide range of amines have been determined. All data obtained, including second‐order kinetics, lack of cross‐over, and negative entropies of activation for reaction of triphenylphosphine borane with quinuclidine and triethylamine, are consistent with a direct (SN2‐like) transfer process, rather than a dissociative (SN1‐like) process. The identities of the amine, phosphine, and solvent all impact substantially on the rate (k) and equilibrium (K) of the transfer, which in some cases vary by many orders of magnitude. P‐to‐N transfer is more efficient with cyclic amines in apolar solvents due to reduced entropic costs and ground‐state destabilisation. Taken as a whole, the data allow informed optimisation of the deprotection step from the stand‐point of rate, or synthetic convenience. In all cases, both reactants should be present at high initial concentration to gain kinetic benefit from the bimolecularity of the process. Ultimately, the choice of amine is dictated by the identity of the phosphine borane complex. Aryl‐rich phosphine boranes are sufficiently reactive to allow use of diethylamine or pyrrolidine as a volatile low polarity solvent and reactant, whereas more alkyl‐rich phosphines benefit from the use of more reactive amines, such as 1,4‐diaza[2.2.2]bicyclooctane (DABCO), in apolar solvents at higher temperatures.  相似文献   

12.
Chiral self-recognition and self-discrimination are of vital importance to biological processes. In this work, 2D regular rhombic nanocrystals ( RS -NC ) were fabricated through heterochiral self-discrimination between chiral polynuclear gold(I)-sulfido complex enantiomers, [(R-BINAP)4Au10S4]Cl2 ( R -Au10 ) and [(S-BINAP)4Au10S4]Cl2 ( S -Au10 ), in MeOH without the need for any surfactants or templates. The monitoring of nanocrystals (NCs) formation by TEM and DLS has uncovered the self-assembly process and shape evolution of the NCs and revealed a screw-dislocation dictated spiral growth of the rhombic NCs. Upon addition of chiral anions, the morphology of the gold NCs was found to change from rhombic to strip and quasi-hexagonal nanosheets, arising from reverse and rotational layer-by-layer stacking to give the bilayer NCs. By applying a high temperature, rhombic gold nanoisland films were obtained from the rhombic NCs. The current study has provided a simple strategy towards the construction of regular geometric 2D NCs as well as their chiral anion-tuned and reverse and rotational stacking-determined morphology change by heterochiral self-discrimination.  相似文献   

13.
The formation of small 1 to 3 nm organic-ligand free metal-oxide nanocrystals (NCs) is essential to utilization of their attractive size-dependent properties in electronic devices and catalysis. We now report that hexaniobate cluster-anions, [Nb6O19]8−, can arrest the growth of metal-oxide NCs and stabilize them as water-soluble complexes. This is exemplified by formation of hexaniobate-complexed 2.4-nm monoclinic-phase CuO NCs ( 1 ), whose ca. 350 Cu-atom cores feature quantum-confinement effects that impart an unprecedented ability to catalyze visible-light water oxidation with no added photosensitizers or applied potentials, and at rates exceeding those of hematite NCs. The findings point to polyoxoniobate-ligand entrapment as a potentially general method for harnessing the size-dependent properties of very small semiconductor NCs as the cores of versatile, entirely-inorganic complexes.  相似文献   

14.
A new strategy for the synthesis of CdS nanocrystals (NCs) within supramolecular self-assembly nanoreactors has been described. The self-assembly nanoreactors were readily constructed through the electrostatic interactions and ion pairs between palmitic acid and the terminal amine groups of hyperbranched polymer. In a chloroform/water two-phase system, aqueous Cd (2+) ions were spontaneously encapsulated into the cavities of self-assembly nanoreactors in chloroform. After reaction with S (2-) ions, the CdS NCs with high stability were obtained. By the addition of excess triethylamine, CdS NCs formed in the self-assembly nanoreactors were transferred from organic phase into aqueous phase. After dialysis and rotorary evaporation, aqueous CdS NCs could be redispersed into chloroform solution containing palmitic acid.  相似文献   

15.
A convenient and rapid procedure has been achieved to immobilize densely packed nanoporous 3D arrays of oleic acid (OLEA)-capped rod-shaped TiO2 nanocrystals (NCs) and nearly spherical Fe2O3 NCs on the surface of micro mechanical cantilever sensors on SU-8. The NCs have been immobilized at room temperature and in the dark on the micro cantilevers before their release. AFM, SEM and XPS investigations attest for an effective and attachment of the NCs on the SU-8 which occurs with not modifying the original morphology and chemical composition of the nano-objects allowing for an effective accomplishment of the cantilever fabrication.  相似文献   

16.
Low‐dimensional metal halides have recently attracted extensive attention owing to their unique structure and photoelectric properties. Herein, we report the colloidal synthesis of all‐inorganic low‐dimensional cesium copper halide nanocrystals (NCs) by adopting a hot‐injection approach. Using the same reactants and ligands, but different reaction temperatures, both 1D CsCu2I3 nanorods and 0D Cs3Cu2I5 NCs can be prepared. Density functional theory indicates that the reduced dimensionality in 1D CsCu2I3 compared to 0D Cs3Cu2I5 makes the excitons more localized, which accounts for the strong emission of 0D Cs3Cu2I5 NCs. Subsequent optical characterization reveals that the highly luminescent, strongly Stokes‐shifted broadband emission of 0D Cs3Cu2I5 NCs arises from the self‐trapped excitons. Our findings not only present a method to control the synthesis of low‐dimensional cesium copper halide nanocrystals but also highlight the potential of 0D Cs3Cu2I5 NCs in optoelectronics.  相似文献   

17.
Cesium lead halide perovskite nanocrystals (NCs) CsPbX3 (X=Cl, Br, and I) have been prominent materials in the last few years due to their high photoluminescence quantum yield (PLQY) for light-emitting diodes and other significant applications in photovoltaics and optoelectronics. In colloidal CsPbX3 synthesis, the most commonly used ligands are oleic acid and oleylamine. The latter plays an important role in surface passivation but may also be responsible for poor colloidal stability as a result of facile proton exchange leading to the formation of labile oleylammonium halide, which pulls halide ions out of the NC surface. Herein, a facile, efficient, completely amine-free synthesis of cesium lead bromide perovskite nanocrystals using hydrobromic acid as halide source and tri-n-octylphosphane as ligand under open-atmospheric conditions is demonstrated. Hydrobromic acid serves as labile source of bromide ion, and thus this three-precursor approach (separate precursors for Cs, Pb, Br) gives more control than a conventional single-source precursor for Pb and Br (PbBr2). The use of HBr paved the way to eliminate oleylamine, and thus the formation of labile oleylammonium halide can be completely excluded. Various Cs:Pb:Br molar ratios were studied and optimum conditions for making very stable CsPbBr3 NCs with high PLQY were found. These completely amine-free CsPbBr3 perovskite NCs synthesized under bromine-rich conditions exhibit good stability and durability for more than three months in the form of colloidal solutions and films, respectively. Furthermore, stable tunable emission across a wide spectral range through anion exchange was demonstrated. More importantly, this work reports open-atmosphere-stable CsPbBr3 NCs films exhibiting strong PL, which can be further used for optoelectronic device applications.  相似文献   

18.
ABX3-type halide perovskite nanocrystals (NCs) have been a hot topic recently due to their fascinating optoelectronic properties. It has been demonstrated that A-site ions have an impact on their photophysical and chemical properties, such as the optical band gap and chemical stability. The pursuit of halide perovskite materials with diverse A-site species would deepen the understanding of the structure–property relationship of the perovskite family. In this work we have attempted to synthesize rubidium-based perovskite NCs. We have discovered that the partial substitution of Rb+ by Cs+ help to stabilize the orthorhombic RbPbBr3 NCs at low temperature, which otherwise can only be obtained at high temperature. The inclusion of Cs+ into the RbPbBr3 lattice results in highly photoluminescent Rb1−xCsxPbBr3 NCs. With increasing amounts of Cs+, the band gaps of the Rb1−xCsxPbBr3 NCs decrease, leading to a redshift of the photoluminescence peak. Also, the Rb1−xCsxPbBr3 NCs (x=0.4) show good stability under ambient conditions. This work demonstrates the high structural flexibility and tunability of halide perovskite materials through an A-site cation substitution strategy and sheds light on the optimization of perovskite materials for application in high-performance optoelectronic devices.  相似文献   

19.
Novel β‐NaGdF4/Na(Gd,Yb)F4:Er/NaYF4:Yb/NaNdF4:Yb core/shell 1/shell 2/shell 3 (C/S1/S2/S3) multi‐shell nanocrystals (NCs) have been synthesized and used as probes for in vivo imaging. They can be excited by near‐infrared (800 nm) radiation and emit short‐wavelength infrared (SWIR, 1525 nm) radiation. Excitation at 800 nm falls into the “biological transparency window”, which features low absorption by water and low heat generation and is considered to be the ideal excitation wavelength with the least impact on biological tissues. After coating with phospholipids, the water‐soluble NCs showed good biocompatibility and low toxicity. With efficient SWIR emission at 1525 nm, the probe is detectable in tissues at depths of up to 18 mm with a low detection threshold concentration (5 nM for the stomach of nude mice and 100 nM for the stomach of SD rats). These results highlight the potential of the probe for the in vivo monitoring of areas that are otherwise difficult to analyze.  相似文献   

20.
The single X-ray crystal structure of the cadmium(II)–S-benzyl dithiocarbazate (SBDTC) complex, [Cd(SBDTC)Cl2]2, is reported. The compound has been found to be an effective single-source precursor for the preparation of CdS nanocrystals (NCs) via solvothermal method. CdS NCs including spheres and rods were prepared at a relatively low temperature by thermolysis of the precursor using chelating solvent like ethylene glycol (EG), ethylenediamine (EN), hydrazine hydrate (HH) or in a mixture of EG and EN. The influence of solvent, temperature and reaction time was investigated on the size and morphology of the NCs. Use of EG afforded spherical CdS NCs while EN uniquely yielded rod-shaped NCs, and mixture of spheres and rods are obtained from the mixture of EN and EG with a ratio 0.2 (v/v: EN/EG). UV–visible spectroscopy established pronounced quantum confinement with enhanced band gap and XRD analyses revealed hexagonal crystal phase for so obtained CdS NCs. The NCs were also characterized by transmission electron microscopy (TEM), photoluminescence spectroscopy (PL), energy-dispersive X-ray spectroscopy (EDS) and FTIR. The possible formation mechanism for the anisotropic growth of NCs was also discussed.  相似文献   

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