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1.
J Phys Chem Lett ; : 4990-4997, 2020 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-32498513

RESUMO

Polar surfaces of ionic crystals are of growing technological importance, with implications for the efficiency of photocatalysts, gas sensors, and electronic devices. The creation of ionic nanocrystals with high percentages of polar surfaces is an option for improving their efficiency in the aforementioned applications but is hard to accomplish because they are less thermodynamically stable and prone to vanish during the growth process. Herein, we develop a strategy that is capable of producing polar surface-dominated II-VI semiconductor nanocrystals, including ZnS and CdS, from copper sulfide hexagonal nanoplates through cation exchange reactions. The obtained wurtzite ZnS hexagonal nanoplates have dominant {002} polar surfaces, occupying up to 97.8% of all surfaces. Density functional theory calculations reveal the polar surfaces can be stabilized by a charge transfer of 0.25 eV/formula from the anion-terminated surface to the cation-terminated surface, which also explains the presence of polar surfaces in the initial Cu1.75S hexagonal nanoplates with cation deficiency prior to cation exchange reactions. Experimental results showed that the HER activity could be boosted by the surface polarization of polar surface-dominated ZnS hexagonal nanoplates. We anticipate this strategy is general and could be used with other systems to prepare nanocrystals with dominant polar surfaces. Furthermore, the availability of colloidal semiconductor nanocrystals with dominant polar surfaces produced through this strategy opens a new avenue for improving their efficiency in catalysis, photocatalysis, gas sensing, and other applications.

2.
Small ; 16(12): e1902231, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31769587

RESUMO

For the first time, colloidal gold (Au)-ZnSe hybrid nanorods (NRs) with controlled size and location of Au domains are synthesized and used for hydrogen production by photocatalytic water splitting. Au tips are found to grow on the apices of ZnSe NRs nonepitaxially to form an interface with no preference of orientation between Au(111) and ZnSe(001). Density functional theory calculations reveal that the Au tips on ZnSe hybrid NRs gain enhanced adsorption of H compared to pristine Au, which favors the hydrogen evolution reaction. Photocatalytic tests reveal that the Au tips on ZnSe NRs effectively enhance the photocatalytic performance in hydrogen generation, in which the single Au-tipped ZnSe hybrid NRs show the highest photocatalytic hydrogen production rate of 437.8 µmol h-1 g-1 in comparison with a rate of 51.5 µmol h-1 g-1 for pristine ZnSe NRs. An apparent quantum efficiency of 1.3% for hydrogen evolution reaction for single Au-tipped ZnSe hybrid NRs is obtained, showing the potential application of this type of cadmium (Cd)-free metal-semiconductor hybrid nanoparticles (NPs) in solar hydrogen production. This work opens an avenue toward Cd-free hybrid NP-based photocatalysis for clean fuel production.

3.
Adv Mater ; 31(49): e1905540, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31631407

RESUMO

Molecular surfactants are widely used to control low-dimensional morphologies, including 2D nanomaterials in colloidal chemical synthesis, but it is still highly challenging to accurately control single-layer growth for 2D materials. A scalable stacking-hinderable strategy to not only enable exclusive single-layer growth mode for transition metal dichalcogenides (TMDs) selectively sandwiched by surfactant molecules but also retain sandwiched single-layer TMDs' photoredox activities is developed. The single-layer growth mechanism is well explained by theoretical calculation. Three types of single-layer TMDs, including MoS2 , WS2 , and ReS2 , are successfully synthesized and demonstrated in solar H2 fuel production from hydrogen-stored liquid carrier-methanol. Such H2 fuel production from single-layer MoS2 nanosheets is COx -free and reliably workable under room temperature and normal pressure with the generation rate reaching ≈617 µmole g-1 h-1 and excellent photoredox endurability. This strategy opens up the feasible avenue to develop methanol-storable solar H2 fuel with facile chemical rebonding actualized by 2D single-layer photocatalysts.

4.
J Phys Chem Lett ; 10(12): 3465-3471, 2019 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-31184156

RESUMO

Herein we employed a first-principles method based on density functional theory to investigate the surface energy and growth kinetics of wurtzite nanoplatelets to elucidate why nanoplatelets exhibit a uniform thickness of eight monolayers. We synthesized a series of wurtzite nanoplatelets (ZnSe, ZnS, ZnTe, and CdSe) with an atomically uniform thickness of eight monolayers. As a representative example, the growth mechanism of 1.39 nm thick (eight monolayers) wurtzite ZnSe nanoplatelets was studied to substantiate the proposed growth kinetics. The results show that the growth of the seventh and eighth layers along the [112̅0] direction of 0.99 nm (six monolayers) ZnSe magic-size nanoclusters is accessible, whereas the growth of the ninth layer is unlikely to occur because the formation energy is large. This work not only gives insights into the synthesis of atomically uniform thick wurtzite semiconductor nanoplatelets but also opens up new avenues to their applications in light-emitting diodes, catalysis, detectors, and lasers.

5.
Adv Mater ; 31(25): e1900781, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31063615

RESUMO

Quasi-1D colloidal semiconductor nanorods (NRs) are at the forefront of nanoparticle (NP) research owing to their intriguing size-dependent and shape-dependent optical and electronic properties. The past decade has witnessed significant advances in both fundamental understanding of the growth mechanisms and applications of these stimulating materials. Herein, the state-of-the-art of colloidal semiconductor NRs is reviewed, with special emphasis on heavy-metal-free materials. The main growth mechanisms of heavy-metal-free colloidal semiconductor NRs are first elaborated, including anisotropic-controlled growth, oriented attachment, solution-liquid-solid method, and cation exchange. Then, structural engineering and properties of semiconductor NRs are discussed, with a comprehensive overview of core/shell structures, alloying, and doping, as well as semiconductor-metal hybrid nanostructures, followed by highlighted practical applications in terms of photocatalysis, photodetectors, solar cells, and biomedicine. Finally, challenges and future opportunities in this fascinating research area are proposed.

6.
Adv Mater ; 30(39): e1803351, 2018 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-30059172

RESUMO

Quasi-1D cadmium chalcogenide quantum rods (QRs) are benchmark semiconductor materials that are combined with noble metals to constitute QR heterostructures for efficient photocatalysis. However, the high toxicity of cadmium and cost of noble metals are the main obstacles to their widespread use. Herein, a facile colloidal synthetic approach is reported that leads to the spontaneous formation of cadmium-free alloyed ZnSx Se1-x QRs from polydisperse ZnSe nanowires by alkylthiol etching. The obtained non-noble-metal ZnSx Se1-x QRs can not only be directly adopted as efficient photocatalysts for water oxidation, showing a striking oxygen evolution capability of 3000 µmol g-1 h-1 , but also be utilized to prepare QR-sensitized TiO2 photoanodes which present enhanced photo-electrochemical (PEC) activity. Density functional theory (DFT) simulations reveal that alloyed ZnSx Se1-x QRs have highly active Zn sites on the (100) surface and reduced energy barrier for oxygen evolution, which in turn, are beneficial to their outstanding photocatalytic and PEC activities.

7.
Chem Asian J ; 12(3): 347-354, 2017 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-27900854

RESUMO

Novel hollow Ag/MnO2 nanostructures with controlled shell composition and structure were designed and synthesized. In the present synthetic procedure, silver nanocrystals were oxidized by KMnO4 , and MnO2 was heterogeneously formed on the surface of silver nanocrystals, then released Ag+ was photoreduced to silver adjacent to MnO2 . By simply changing the photoreduction moment, simultaneously with or after the addition of KMnO4 , hollow Ag/MnO2 structures with different shell architectures-a monolayered shell composed of evenly mixed silver and MnO2 and a double-layered shell composed of an inner MnO2 layer and an outer silver layer-can be obtained. Furthermore, the morphology of the hollow structure can be tuned by selecting different silver precursors, and the ratio of silver to MnO2 in the shell can also be controlled by adjusting the ratio in the original reaction mixture. Electrochemical measurements revealed significantly enhanced catalytic performance in the oxygen reduction reaction for the prepared hollow structures. Compared with the Ag/MnO2 composite, the onset potentials positively shift by about 50.0 mV and limiting current densities are nearly 2.0 times higher.

8.
Chemistry ; 22(27): 9321-9, 2016 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-27219903

RESUMO

A facile liquid-phase exfoliation method to prepare few-layer FeOCl nanosheets in acetonitrile by ultrasonication is reported. The detailed exfoliation mechanism and generated products were investigated by combining first-principle calculations and experimental approaches. The similar cleavage energies of FeOCl (340 mJ m(-2) ) and graphite (320 mJ m(-2) ) confirm the experimental exfoliation feasibility. As a Fenton reagent, FeOCl nanosheets showed outstanding properties in the catalytic degradation of phenol in water at room temperature, under neutral pH conditions, and with sunlight irradiation. Apart from the increased surface area of the nanosheets, the surface state change of the nanosheets also plays a key role in improving the catalytic performance. The changes of charge density, density of states (DOS), and valence state of Fe atoms in the exfoliated FeOCl nanosheets versus plates illustrated that surface atomistic relationships made the few-layer nanosheets higher activity, indicating the exfoliation process of the FeOCl nanosheets also brought about surface state changes.

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