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1.
Small ; 20(5): e2304822, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37726224

RESUMEN

The generation of an active phase through dynamic surface reconstruction is a promising strategy for improving the activity of electrocatalysts. However, studies investigating the reconstruction process and its impact on the intrinsic properties of the catalysts are scarce. Herein, the surface reconstruction of NiFe2 O4 interfaced with NiMoO4 (Ru-NFO/NMO) facilitated by Ru doping is reported. The electrochemical and material characterizations demonstrate that Ru doping can regulate the electronic structure of NFO/NMO and induce the high-valence state of Ni3.6+ δ , facilitating the surface reconstruction to highly active Ru-doped NiFeOOH/NiOOH (SR-Ru-NFO/NMO). The optimized SR-Ru-NFO/NMO exhibits promising performance in the oxygen evolution reaction, displaying a low overpotential of 229 mV at 10 mA cm-2 and good stability at varying current densities for 80 h. Density functional theory calculations indicate that Ru doping can increase the electron density and optimize intermediate adsorption by shifting the d-band center downward. This work provides valuable insights into the tuning of electrocatalysts by surface reconstruction and offers a rational design strategy for the development of highly active oxygen evolution reaction electrocatalysts.

2.
Small Methods ; 5(7): e2100215, 2021 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-34928005

RESUMEN

The use of a conducting interlayer between separator and cathode is one of the most promising methods to trap lithium polysulfides (LiPSs) for enhancing the performance of lithium-sulfur (Li-S) batteries. Red phosphorus nanoparticles (RPEN )-coated carbon nanotube (CNT) film (RPEN @CF) is reported herein as a novel interlayer for Li-S batteries, which shows strong chemisorption of LiPSs, good flexibility, and excellent electric conductivity. A pulsed laser ablation method is engaged for the ultrafast production of RPEN of uniform morphology, which are deposited on the CNT film by a direct spinning method. The RPEN @CF interlayer provides pathways for effective Li+ and electron transfer and strong chemical interaction with LiPSs. The S/RPEN @CF electrode shows a superior specific capacity of 782.3 mAh g-1 (3 C-rate) and good cycling performances (769.5 mAh g-1 after 500 cycles at 1 C-rate). Density functional theory calculations reveal that the morphology and dispersibility of RPEN are crucial in enhancing Li+ and electron transfer kinetics and effective trap of LiPSs. This work demonstrates the possibility of using the RPEN @CF interlayer for the enhanced electrochemical performances of Li-S batteries and other flexible energy storage devices.

3.
ACS Appl Mater Interfaces ; 13(8): 9762-9770, 2021 Mar 03.
Artículo en Inglés | MEDLINE | ID: mdl-33605144

RESUMEN

Transition metal phosphosulfides (TMPSs) have gained much interest due to their highly enhanced photocatalytic activities compared to their corresponding phosphides and sulfides. However, the application of TMPSs on photocatalytic CO2 reduction remains a challenge due to their inappropriate band positions and rapid recombination of photogenerated electron-hole pairs. Herein, we report ultrasmall copper phosphosulfide (us-Cu3P|S) nanocrystals anchored on 2D g-C3N4 nanosheets. Systematic studies on the interaction between us-Cu3P|S and g-C3N4 indicate the formation of an S-scheme heterojunction via interfacial P-N chemical bonds, which acts as an electron transfer channel and facilitates the separation and migration of photogenerated charge carriers. Upon the composite formation, the band structures of us-Cu3P|S and g-C3N4 are altered to enable the enhanced photocatalytic CO generation rate of 137 µmol g-1 h-1, which is eight times higher than that of pristine g-C3N4. The unique phosphosulfide structure is also beneficial for the enhanced electron transfer rate and provides abundant active sites. This first application of Cu3P|S to photocatalytic CO2 reduction marks an important step toward the development of TMPSs for photocatalytic applications.

4.
ACS Appl Mater Interfaces ; 12(19): 21944-21951, 2020 May 13.
Artículo en Inglés | MEDLINE | ID: mdl-32319744

RESUMEN

Solution-processable perovskite quantum dots are considered as promising optical materials for light-emitting optoelectronics. Light-emitting field-effect transistors (LEFETs) that can be operated under a relatively lower potential with a high energy conversion efficiency are yet to be realized with perovskite quantum dots. Here, we present the CsPbBr3 quantum dot-based LEFET. Surprisingly, unipolar transport characteristics with strong electroluminescence were observed at the interface of the CsPbBr3 QD-LEFET along with an exceptionally wide recombination zone of 80 µm, an order of magnitude larger than that of organic/polymer LEFETs. Based on the systematic analysis for the electroluminescence of the CsPbBr3 NC-LEFET, we revealed that the increased diffusion length determined by the majority carrier mobility and the lifetime well explains the remarkably wide recombination zone. Furthermore, it was found that the energy-level matching and transport geometry of the heterostructure also determine the charge distribution and recombination, substantially affecting the performance of the CsPbBr3 QD LEFET.

5.
ACS Appl Mater Interfaces ; 8(36): 23676-87, 2016 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-27538809

RESUMEN

We demonstrate stable hybrid electrochemical energy storage performance of a redox-active electrolyte, namely potassium ferricyanide in aqueous media in a supercapacitor-like setup. Challenging issues associated with such a system are a large leakage current and high self-discharge, both stemming from ion redox shuttling through the separator. The latter is effectively eliminated when using an ion exchange membrane instead of a porous separator. Other critical factors toward the optimization of a redox-active electrolyte system, especially electrolyte concentration and volume of electrolyte, have been studied by electrochemical methods. Finally, excellent long-term stability is demonstrated up to 10 000 charge/discharge cycles at 1.2 and 1.8 V, with a broad maximum stability window of up to 1.8 V cell voltage as determined via cyclic voltammetry. An energy capacity of 28.3 Wh/kg or 11.4 Wh/L has been obtained from such cells, taking the nonlinearity of the charge-discharge profile into account. The power performance of our cell has been determined to be 7.1 kW/kg (ca. 2.9 kW/L or 1.2 kW/m(2)). These ratings are higher compared to the same cell operated in aqueous sodium sulfate. This hybrid electrochemical energy storage system is believed to find a strong foothold in future advanced energy storage applications.

6.
Opt Lett ; 34(18): 2745-7, 2009 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-19756091

RESUMEN

We report a type of hybrid optical fiber created by filling the central hole of a silica hollow optical fiber (HOF) with an organic polymer to serve as the core. After suitable curing of the polymer filling of the HOF, a self-assembled one-dimensional polymer-air periodic structure was created without the need for an amplitude mask. This acts as a long-period fiber grating device with an axial refractive index modulation. Details of the fabrication method for the hybrid fiber grating and its transmission spectra analysis are reported.

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