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2.
Front Chem ; 10: 1050046, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36385984

RESUMEN

We designed an edge-sites 2D/0D/2D based TiO2@Au/g-C3N4 Z-scheme photocatalytic system consists of highly exposed (001) TNSs@Au edge-site heterojunction, and the Au/g-C3N4 interfacial heterojunction. The designed photocatalyst was prepared by a facile and controlled hydrothermal synthesis strategy via in-situ nanoclusters-to-nanoparticles deposition technique and programable calcination in N2 atmosphere to get edge-site well-crystalline interface, followed by chemically bonded thin overlay of g-C3N4. Photocatalytic performance of the prepared TNSs@Au/g-C3N4 catalyst was evaluated by the photocatalytic degradation of organic pollutants in water under visible light irradiation. The results obtained from structural and chemical characterization conclude that the inter-facet junction between highly exposed (001) and (101) TNSs surface, and TNSs@Au interfacial heterojunction formed by a direct contact between highly crystalline TNSs and Au, are the key factors to enhance the separation efficiency of photogenerated electrons/holes. On coupling with overlay of g-C3N4 2D NSs synergistically offer tremendous reactive sites for the potential photocatalytic dye degradation in the Z-scheme photocatalyst. Particularly in the designed photocatalyst, Au nanoparticles accumulates and transfer the photo-stimulated electrons originated from anatase TNSs to g-C3N4 via semiconductor-metal heterojunction. Because of the large exposed reactive 2D surface, overlay g-C3N4 sheets not only trap photoelectrons, but also provide a potential platform for increased adsorption capacities for organic contaminants. This work establishes a foundation for the development of high-performance Z-scheme photocatalytic systems.

3.
Adv Sci (Weinh) ; 9(18): e2200346, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35466563

RESUMEN

The construction of photocatalytic systems that have strong redox capability, effective charge separation, and large reactive surfaces is of great scientific and practical interest. Herein, an edge-connected 2D/2D Z-scheme system that combines the facet junction and the interfacial heterojunction to achieve effective long-range charge separation and large reactive surface exposure is designed and fabricated. The heterostructure is realized by the selective growth of 2D-layered MoS2 nanoflakes on the edge-sites of thin TiO2 nanosheets via an Au-promoted photodeposition method. Attributed to the synergetic coupling of the facet junction and the interfacial heterojunction that assures the effective charge separation, and the tremendous but physically separated reactive sites offered by layered MoS2 and highly-exposed (001) facets of TiO2 , respectively, the artificial Z-scheme exhibits excellent photocatalytic performance in photodegradation tests. Moreover, the junctional plasmonic Au nanoclusters not only act as electron traps to promote the edge-selective synthesis but also generate "hot electrons" to further boost photocatalytic performance. The Z-scheme charge-flow direction in the heterostructure and the roles of electrons and holes are comprehensively studied using in situ irradiated X-ray photoelectron spectroscopy and photodegradation tests. This work offers a new insight into designing high-performance Z-scheme photocatalytic systems.

4.
Langmuir ; 36(31): 9284-9290, 2020 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-32674576

RESUMEN

We reported a controlled synthesis method to obtained carbon spheres with tunable geometry under low ZnCl2 aqueous solution conditions using polytriazine as a precursor. The polytriazine precursor was polymerized by mixing/reaction of 2,6-diaminopyridine and formaldehyde in the presence of a diluted ZnCl2 aqueous system. The obtained nanospheres were then decomposed to adulterate nitrogen porous carbon nanospheres (N-PCNSs) by the decomposition and blistering process at high temperature by degrees. ZnCl2 worked as a solid-template and played the role of a stabilizing and foaming agent in the reaction. The as-prepared N-PCNSs with controllable spherical geometry, large micro-/mesoporous volume and high nitrogen content (∼8.5 wt %) were employed in electric double-layer capacitors that have a good specific capacitance (636 F/g at 1 A/g) and are long lasting. Besides, the N-PCNS delivered a high energy density of 22.1 Wh/Kg at a power density of 500 W/kg.

5.
Nanotechnology ; 31(39): 395704, 2020 Sep 25.
Artículo en Inglés | MEDLINE | ID: mdl-32434169

RESUMEN

As the most representative member of a new emerging family of 2D material, titanium carbides or nitrides (MXenes), Ti3C2Tx and its 2D assembly format, Ti3C2Tx film, have displayed outstanding performance in a broad range of practical applications. However the mechanical behaviors of Ti3C2Tx films are rarely reported. We report a systematic study of the tensile behavior of Ti3C2Tx films. Ti3C2Tx films with various thicknesses (2-17 µm) were prepared by the vacuum filtration method. Quasi-static tension and cyclic tension tests were performed to investigate the deformation and fracture mechanism of Ti3C2Tx films. It was found that: (1) the relative sliding between Ti3C2Tx flakes is the dominant deformation mechanism of Ti3C2Tx films. Cyclic loading-releasing in tension suppresses the inter-layer sliding of Ti3C2Tx flakes effectively and thus the tensile strength of thicker Ti3C2Tx film (5 µm) film improves from 57 MPa to 67 MPa. (2) The mechanical properties of Ti3C2Tx films are found to be thickness dependent. When the film thickness increases from 2.3 to 17 µm, the tensile strength and elastic modulus drop from 61 to 36 MPa and from 17 to 8 GPa, respectively. This is interpreted as more structural defects presented in the through-the-thickness direction as film thickness is increased. (3) Moderate ultrasonication pretreatment (30 min) reduces the Ti3C2Tx flake size significantly while improving the compactness of the Ti3C2Tx film; and the resulting Ti3C2Tx film shows a linear stress-strain relationship without plastic-like deformation. As a result, the tensile strength of 5 µm thick Ti3C2Tx film is enhanced to 85 MPa; (4) Structural defects of the Ti3C2Tx film have significant effects on both the brittle-like fracture behavior and the distribution of tensile strength.

6.
Nanotechnology ; 31(12): 125708, 2020 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-31796652

RESUMEN

Improving Schottky diode characteristics in semiconducting devices is essential for better functionality in electronic and optoelectronic devices at nanoscale. In this paper, we investigate the electric transport characteristics of a gold (Au)-tip/n-Si-based nano-Schottky diode by using a conductive-mode atomic force microscope (CAFM). First, 10 nm average diameter Au nanoparticles (NPs) are monodispersed on the highly cleaned n-type Si substrate using an optimized spin-coating technique. The controlled and well dispersed NPs are confirmed by using the AC imaging mode of the AFM. The electrical characteristics are established by using an Au-coated AFM tip, by either soft engaging at the surface of the n-Si substrate or at the top of an individual Au NP. Landing of the AFM tip on the NP or n-Si substrate is validated by the force curves of the AFM. From the localized CAFM electrical characteristics, we observed the improvement in the figures of merit (FOM) that characterize the rectification performance including the (1-V) asymmetry (f ASYM), and the turn-on voltage due to placing the Au NP between the AFM tip and n-Si substrate. These improved FOM of the nanoscale diodes are explained based on the increase in the tunneling current at the nanoscale Au-NP/n-Si interface. Moreover, the nanoscale control of interface structure is extremely important to improve the characteristics of nano-Schottky diodes.

7.
ACS Appl Mater Interfaces ; 11(25): 22323-22331, 2019 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-31149805

RESUMEN

In response to the increasing concern for energy management, molybdenum disulfide (MoS2) has been extensively researched as an attractive anode material for sodium-ion batteries (SIBs). The proficient cycling durability and good rate performance of SIBs are the two key parameters that determine their potential for practical use. In this study, nature-inspired three-dimensional (3D) MoS2 ultrathin marigold flower-like microstructures were prepared by a controlled hydrothermal method. These microscale flowers are constructed by arbitrarily arranged but closely interconnected two-dimensional ultrathin MoS2 nanosheets. The as-prepared MoS2 microflowers (MFs) have then been chemically wrapped by layered graphene sheets to form the bonded 3D hybrid MoS2-G networks. TEM, SEM, XRD, XPS, and Raman characterizations were used to study the morphology, crystallization, chemical compositions, and wrapping contact between MoS2 and graphene. The ultrathin nature of MoS2 in 3D MFs and graphene wrapping provide strong electrical conductive channels and conductive networks in an electrode. Benefitting from the 2 nm ultrathin crystalline MoS2 sheets, chemically bonded graphene, defect-induced sodium storage active sites, and 3D interstitial spaces, the prepared electrode exhibited an outstanding specific capacity (606 mA h g-1 at 200 mA g-1), remarkable rate performance (345 mA h g-1 at 1600 mA g-1), and long cycle life (over 100 cycles with tremendous Coulombic efficiencies beyond 100%). The proposed synthesis strategy and 3D design developed in the present study reveal a unique way to fabricate promising anode materials for SIBs.

8.
Sci Rep ; 8(1): 5718, 2018 Apr 09.
Artículo en Inglés | MEDLINE | ID: mdl-29632316

RESUMEN

In this present study, we report the synthesis of Au nanodots on α-Fe2O3@reduced graphene oxide (RGO) based hetero-photocatalytic nanohybrids through a chlorophyll mediated photochemical synthesis. In this process, chlorophyll induces a rapid reduction (30 min) of Au3+ ions to Au° metallic nanodots on α-Fe2O3@RGO surface under sunlight irradiation. The nucleation growth process, photo-induced electron-transfer mechanism and physico-chemical properties of the Au@α-Fe2O3@RGO ternary nanocomposites were systematically studied with various analytical techniques. This novel photochemical synthesis process is a cost-effective, convenient, surfactant-less, and scalable method. Moreover, the prepared ternary nanocomposites enhanced catalytic activity as compared to pure α-Fe2O3 and α-Fe2O3@RGO. The advantages and synergistic effect of Au@α-Fe2O3@RGO exhibit, (i) a broader range of visible-light absorption due to visible light band gap of α-Fe2O3, (ii) lower recombination possibility of photo-generated electrons and holes due to effect of Au and (iii) faster electron transfer due to higher conductivity of RGO. Therefore, the prepared Au@α-Fe2O3@RGO hetero-photocatalytic nanohybrids exhibited a remarkable photocatalytic activity, thus enabling potential active hetero-photocatalyst for industrial and environmental applications.

9.
ACS Appl Mater Interfaces ; 9(13): 11669-11677, 2017 Apr 05.
Artículo en Inglés | MEDLINE | ID: mdl-28300389

RESUMEN

Low cycling stability and poor rate performance are two of the distinctive drawbacks of most electrode materials for sodium-ion batteries (SIBs). Here, inspired by natural flower structures, we take advantage of the three-dimensional (3D) hierarchical flower-like stable microstructures formed by two-dimensional (2D) nanosheets to solve these problems. By precise control of the hydrothermal synthesis conditions, a novel three-dimensional (3D) flower-like architecture consisting of 2D Na2Ti3O7 nanosheets (Na-TNSs) has been successfully synthesized. The arbitrarily arranged but closely interlinked thin nanosheets in carnation-shaped 3D Na2Ti3O7 microflowers (Na-TMFs) originate a good network of electrically conductive paths in an electrode. Thus, Na-TMFs can get electrons from all directions and be fully utilized for sodium-ion insertion and extraction reactions, which can improve sodium storage properties with enhanced rate capability and super cycling performance. Furthermore, the large specific surface area provides a high capacity, which can be ascribed to the pseudo-capacitance effect. The wettability of the electrolyte was also improved by the porous and crumpled structure. The remarkably improved cycling performance and rate capability of Na-TMFs make a captivating case for its development as an advanced anode material for SIBs.

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