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1.
J Am Chem Soc ; 141(8): 3480-3488, 2019 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-30714725

RESUMO

As crystalline semiconductor nanowires are thinned down to a single-unit-cell thickness, many fascinating properties could arise pointing to promising applications in various fields. A grand challenge is to be able to controllably synthesize such ultrathin nanowires. Herein, we report a strategy, which synergizes a soft template with oriented attachment (ST-OA), to prepare high-quality single-unit-cell semiconductor nanowires (SSNWs). Using this protocol, we are able to synthesize for the first time ZnS and ZnSe nanowires (NWs) with only a single-unit-cell thickness (less than 1.0 nm) and a cluster-like absorption feature (i.e., with a sharp, strong, and significantly blue-shifted absorption peak). Particularly, the growth mechanism and the single-unit-cell structure of the as-prepared ZnS SSNWs are firmly established by both experimental observations and theoretical calculations. Thanks to falling into the extreme quantum confinement regime, these NWs are found to only absorb the light with wavelengths shorter than 280 nm (i.e., solar-blind UV absorption). Utilizing such a unique property, self-powered photoelectrochemical-type photodetectors (PEC PDs) based on the ZnS SSNWs are successfully fabricated. The PDs after interface modification with TiO2 exhibit an excellent solar-blind UV photoresponse performance, with a typical on/off ratio of 6008, a detectivity of 1.5 × 1012 Jones, and a responsivity of 33.7 mA/W. This work opens the door to synthesizing and investigating a new dimension of nanomaterials with a wide range of applications.

2.
Phys Chem Chem Phys ; 18(46): 31410-31418, 2016 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-27748477

RESUMO

SiO2, an insulator, hardly has any photocatalytic acitivity due to its intrinsic property, and it is generally used as a hard template to increase the surface area of catalysts. However, in this work, we found that the surface state of the insulator SiO2 can promote the migration of photogenerated charge carriers, leading to the enhancement of the photooxidation ability of graphitic carbon nitride (g-C3N4). A one-pot calcination method was employed to prepare g-C3N4/SiO2 composites using melamine and SiO2 as precursors. The composites present considerably high photocatalytic degradation activities for 2,4-dichlorophenol (2,4-DCP) and rhodamine B (RhB) under visible light (λ > 420 nm) irradiation, which are about 1.53 and 4.18 times as high as those of bulk g-C3N4, respectively. The enhancement of the photocatalytic activity is due to the fact that the introduction of the insulator SiO2 in g-C3N4/SiO2 composites can greatly improve the specific surface area of the composites; more importantly, the impurity energy level of SiO2 can help accelerate the separation and transfer of electron-hole pairs of g-C3N4. Electron paramagnetic resonance (EPR) spectroscopy and trapping experiments with different radical scavengers show that the main active species of g-C3N4 are superoxide radicals, while holes also play a role in photodegradation. For g-C3N4/SiO2-5, besides superoxide radicals and holes, the effect of hydroxyl radicals was greatly improved. Finally, a possible mechanism for the photogenerated charge carrier migration of the g-C3N4/SiO2 photocatalyst was proposed.

4.
Nanomaterials (Basel) ; 9(2)2019 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-30736439

RESUMO

Benefiting from their ultra-small diameters and highly structural anisotropies, ultrathin semiconductor nanowires (USNWs) are well-known for their fascinating physical/chemical properties, as well as their promising applications in various fields. However, until now, it remains a challenge to synthesize high-quality USNWs with well-controlled diameters and lengths, let alone the exploration of their size-dependent properties and applications. To solve such a challenge, we report herein a ligand-induced low-temperature precursor thermolysis route for the controlled preparation of ultrathin ZnS nanowires, which is based on the oriented assembly of the in-situ formed ZnS clusters/tiny particles. Optimized synthetic conditions allowed the synthesis of ZnS nanowires with a diameter down to 1.0 nm and a length approaching 330 nm. The as-prepared ultrathin ZnS nanowires were then intensively examined by morphological, spectroscopic and electrochemical analytical means to explore their size-dependent optical absorption properties, photocatalytic activities and band-edge energy levels, as well as their underlying growth mechanism. Notably, these USNWs, especially for the thinnest nanowires, were identified to possess an excellent performance in both the selective absorption of ultraviolet (UV) light and photocatalytic degradation of dyes, thus enabling them to serve as longpass ultraviolet filters and high-efficiency photocatalysts, respectively. For the ultrathin ZnS nanowires with a diameter of 1.0 nm, it was also interesting to observe that their exciton absorption peak positions were kept almost unchanged during the continuous extension of their lengths, which has not been reported previously.

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