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1.
J Hazard Mater ; 454: 131531, 2023 07 15.
Artigo em Inglês | MEDLINE | ID: mdl-37146334

RESUMO

Herein, we developed a multimodal antibacterial nanoplatform via synergism effect including knife-effect, photothermal, photocatalytic induced reactive oxygen species (ROS), and Cu2+ inherent attribute. Typically, 0.8-TC/Cu-NS possesses higher photothermal property with the higher photothermal conversion efficiency of 24% and the moderate temperature up to 97 °C. Meanwhile, 0.8-TC/Cu-NS exhibits the more active ROS, 1O2 and ·O2-. Hence, 0.8-TC/Cu-NS possesses best antibacterial properties against S. aureus and E. coli in vitro with efficiency of 99.94%/99.97% under near-infrared (NIR) light, respectively. In the therapeutic practical use for wound healing of Kunming mice, this system exhibits outstanding curing capacity and good biocompatibility. Based on the electron configuration measurement and density functional theory (DFT) simulation, it is confirmed that the electrons on CB of Cu-TCPP flow fleetingly to MXene trough the interface, with redistribution of charge and band upward bending over Cu-TCPP. As a result, the self-assembled 2D/2D interfacial Schottky junction have made great favor to accelerate photogenerated charges mobility, hamper charge recombination, and increases the photothermal/photocatalytic activity. This work gives us a hint to mostly design the multimodal synergistic nanoplatform under NIR light in biological applications without drug resistance.


Assuntos
Escherichia coli , Staphylococcus aureus , Camundongos , Animais , Teoria da Densidade Funcional , Espécies Reativas de Oxigênio/farmacologia , Antibacterianos/farmacologia , Cicatrização
2.
Chem Commun (Camb) ; 58(67): 9373-9376, 2022 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-35920106

RESUMO

The non-uniform plating-stripping behaviours of Li metal anodes hinder the application of Li metal batteries. Here, a stable 3D matrix is designed by coating a carbon skeleton with MXene, and the significant influence of the crystallographic texture of Li metal on electrochemical behaviour is investigated. The results demonstrate that the 3D MXene/carbon skeleton can effectively induce the evolution of advantageous Li(110) facets with a dendrite-free anode interface. Consequently, the modified Li metal anodes deliver stable plating-stripping behaviours.

3.
Small Methods ; 6(7): e2200308, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35661441

RESUMO

Herein, the obtained Cu0.5 Co0.5 -ZIF@Fe2 O3 @CC-150 heterojunction (termed as Cu1- x Cox -ZFC-150) showed high hydrogen and oxygen evolution reaction (HER and OER) activities with low overpotential small Tafel slope. When employed to be the bifunctional anode and cathode, they only needed a cell voltage of 1.62 V. The composite also exhibited excellent photocatalytic performance on CO2 evolution into CO and CH4 . The enhanced OER kinetics and Z-scheme charge transfer model for photocatalytic property have been discussed based on the experiments and density functional theory (DFT) analysis. The optimized phase interfaces, abundant active sites, optional oxygen vacancy, and adjusted Gibbs free energy were beneficial for the fast electron/ion transport enhancing the water splitting performance.

4.
J Colloid Interface Sci ; 606(Pt 2): 1745-1757, 2022 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-34500172

RESUMO

Herein, the optional and controllable growth of Bi2S3 onto NH2-MIL-125 via covalent conjunction strategy was reported. The experimental results demonstrate that the obtained heterojunction exhibits boosting photocatalytic reduction CO2 and organic dye degradation. The 18-Bi2S3@NH2-MIL-125-SH displays the highest yield of 12.46 µmol g-1h-1 of CO, >13 times that of pure NH2-MIL-125. Meanwhile, the reaction kinetic of 18-Bi2S3@NH2-MIL-125-SH in the degradation of methylene blue is uppermost, which is 160 times than that of the commercial P25. The enhancement of photocatalytic performance could be ascribed to the covalent coordination-driven intimate interfacial interaction in n-scheme heterojunction. Meanwhile, the plausible mechanism was also investigated by UV-vis diffuse reflectance (UV-vis), photoluminescence (PL), electrochemical photocurrent, electron spin resonance (ESR) and electrochemical impedance spectroscopy (EIS).


Assuntos
Dióxido de Carbono , Titânio , Catálise , Luz
5.
J Colloid Interface Sci ; 608(Pt 3): 3192-3203, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-34801238

RESUMO

CsPbBr3 quantum dots (CPB QDs) have great potential in photoreduction of CO2 to chemical fuels. However, the low charge transportation efficiency and chemical instability of CPB QDs presents a considerable challenge. Herein, we describe the electrostatic assemblies of negatively charged colloidal two dimensional (2D) Cu-Tetrakis(4-carboxyphenyl) porphyrins (Cu-TCPP) nanosheets and positively CPB QDs to construct the hydride heterojunction. The photogenerated electron migration from CPB QDs to Cu-TCPP nanosheets has been witnessed, providing the supply of long-lived electrons for the reduction of CO2 molecules adsorbed on Cu-TCPP matrix. As a direct result, The CPB@Cu-TCPP-x (x wt% of CPB QDs) photocatalysts exhibit significantly enhanced photocatalytic conversion of CO2, compared to the parent Cu-TCPP nanosheets or single CPB QDs. Especially, when with 20% CPB QDs, the heterostruture system achieves an evolution yield of 287.08 µmol g-1 in 4 h with highly CO selectivity (99%) under visible light irradiation, which is equivalent to a 3.87-fold improvement compared to the pristine CPB QDs. Meanwhile, the CH4 generation rate can be up to 3.25 µmol g-1. This optimized construction of heterostructure could provide a platform to funnel photoinduced electrons to the reaction center, which can both act as a crucial capture and the reaction actives of CO2.

6.
Chemistry ; 24(39): 9976-9982, 2018 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-29683534

RESUMO

The synthesis of luminescent polyoxometalates (POMs) typically relies on the assembly of POM ligands with rare earth or transition metals, placing significant constraints on the composition, structure, and hence the luminescence properties of the resultant systems. Herein, we show that the ion-exchange strategy can be used for the synthesis of novel POM-based luminescent materials. We demonstrate that introducing bismuth ions into an ion-exchangeable, microporous POM compound yields an unconventional system luminescing in the near-infrared region. Experimental characterization, coupled with quantum chemical calculations, confirms that bismuth ions site-specifically occupy an off-center site in the lattice, and have an asymmetric coordination geometry unattainable by other means, thus giving rise to peculiar emission. Our findings offer an effective strategy for the synthesis of POM-based luminescent materials, and the design concept may potentially be adapted to the creation of POM-based systems with other functionalities.

7.
Dalton Trans ; 47(3): 684-692, 2018 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-29099525

RESUMO

Visible-light-driven organic transformations have received much attention because of their low cost, relative safety, and environmental friendliness. In this work, we report a series of Bi2S3@ZIF-8 core-shell heterostructures prepared using a simple and efficient self-assembly process. The photocatalytic activity was evaluated using the photocatalytic degradation of Rhodamine B (RhB) under visible-light irradiation and the results show that the core-shell Bi2S3@ZIF-8 heterostructure can remarkably enhance the photocatalytic efficiency at room temperature compared to pristine Bi2S3 nanorods. In addition, the Bi2S3@ZIF-8 composite with a Bi/Zn molar ratio of 1/10 demonstrates good structural stability after the degradation experiment and its photocatalytic activity remains at about 95% after the five recycling tests. The improved photocatalytic performance can be attributed to the larger specific surface area, increased light absorption, and more efficient separation of photogenerated electron-hole pairs due to the combined effects of Bi2S3 and ZIF-8. Moreover, the synergistic photocatalysis mechanism was investigated.

8.
J Phys Chem Lett ; 7(14): 2735-41, 2016 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-27377481

RESUMO

Doping of semiconductors by introducing foreign atoms enables their widespread applications in microelectronics and optoelectronics. We show that this strategy can be applied to direct bandgap lead-halide perovskites, leading to the realization of ultrawide photoluminescence (PL) at new wavelengths enabled by doping bismuth (Bi) into lead-halide perovskites. Structural and photophysical characterization reveals that the PL stems from one class of Bi doping-induced optically active center, which is attributed to distorted [PbI6] units coupled with spatially localized bipolarons. Additionally, we find that compositional engineering of these semiconductors can be employed as an additional way to rationally tune the PL properties of doped perovskites. Finally, we accomplished the electroluminescence at cryogenic temperatures by using this system as an emissive layer, marking the first electrically driven devices using Bi-doped photonic materials. Our results suggest that low-cost, earth-abundant, solution-processable Bi-doped perovskite semiconductors could be promising candidate materials for developing optical sources operating at new wavelengths.

9.
Angew Chem Int Ed Engl ; 55(16): 4967-71, 2016 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-26971863

RESUMO

A low-temperature topochemical reduction strategy is used herein to prepare unconventional phosphors with luminescence covering the biological and/or telecommunications optical windows. This approach is demonstrated by using Bi(III)-doped Y2O3 (Y(2-x)Bi(x)O3) as a model system. Experimental results suggest that topochemical treatment of Y(2-x)Bi(x)O3 using CaH2 creates randomly distributed oxygen vacancies in the matrix, resulting in the change of the oxidation states of Bi to lower oxidation states. The change of the Bi coordination environments from the [BiO6] octahedra in Y(2-x)Bi(x)O3 to the oxygen-deficient [BiO(6-z)] polyhedra in reduced phases leads to a shift of the emission maximum from the visible to the near-infrared region. The generality of this approach was further demonstrated with other phosphors. Our findings suggest that this strategy can be used to explore Bi-doped or other classes of luminescent systems, thus opening up new avenues to develop novel optical materials.

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