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1.
Small ; : e2311770, 2024 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-38794870

RESUMO

Developing low-cost and highly efficient bifunctional catalysts for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) is a challenging problem in electrochemical overall water splitting. Here, iron, tungsten dual-doped nickel sulfide catalyst (Fe/W-Ni3S2) is synthesized on the nickel foam, and it exhibits excellent OER and HER performance. As a result, the water electrolyze based on Fe/W-Ni3S2 bifunctional catalyst illustrates 10 mA cm-2 at 1.69 V (without iR-compensation) and highly durable overall water splitting over 100 h tested under 500 mA cm-2. Experimental results and DFT calculations indicate that the synergistic interaction between Fe doping and Ni vacancy induced by W leaching during the in situ oxidation process can maximize exposed OER active sites on the reconstructed NiOOH species for accelerating OER kinetics, while the Fe/W dual-doping optimizes the electronic structure of Fe/W-Ni3S2 and the binding strength of intermediates for boosting HER. This study unlocks the different promoting mechanisms of incorporating Fe and W for boosting the OER and HER activity of Ni3S2 for water splitting, which provides significant guidance for designing high-performance bifunctional catalysts for overall water splitting.

2.
ACS Nano ; 14(8): 9807-9818, 2020 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-32709197

RESUMO

The abundant reserve and low price of potassium resources promote K-ion batteries (KIBs) becoming a promising alternative to Li-ion batteries, while the large ionic radius of K-ions creates a formidable challenge for developing suitable electrodes. Here Ni-substituted Prussian blue analogues (PBAs) are investigated comprehensively as cathodes for KIBs. The synthesized K1.90Ni0.5Fe0.5[Fe(CN)6]0.89·0.42H2O (KNFHCF-1/2) takes advantage of the merits of high capacity from electrochemically active Fe-ions, outstanding electrochemical kinetics induced by decreased band gap and K-ion diffusion activation energy, and admirable structure stability from inert Ni-ions. Therefore, a high first capacity of 81.6 mAh·g-1 at 10 mA·g-1, an excellent rate property (53.4 mAh·g-1 at 500 mA·g-1), and a long-term lifespan over 1000 cycles with the lowest fading rate of 0.0177% per cycle at 100 mA·g-1 can be achieved for KNFHCF-1/2. The K-ion intercalation/deintercalation proceeds through a facile solid solution mechanism, allowing 1.5-electron transfer based on low- and high-spins FeII/FeIII couples, which is verified by ex situ XRD, XPS, and DFT calculations. The K-ion full battery is also demonstrated using a graphite anode with a high energy density of 282.7 Wh·kg-1. This work may promote more studies on PBA electrodes and accelerate the development of KIBs.

3.
J Colloid Interface Sci ; 538: 286-296, 2019 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-30529841

RESUMO

Over the past decade, there has been increasing interest in the use of multifunctional nanoparticles (NPs) for cancer treatment. Of importance are systems that can deliver drugs at a sustained rate to target cancer cells, which can result in higher efficiency and reduced systemic toxicity. In this study, we present the route for the synthesis of tantalum pentoxide (Ta2O5) NPs with a particle size of 27 nm that were individually coated with poly(acrylic acid) (PAA) with a different layer thickness of 2-8 nm by in-situ polymerization of the acrylic acid monomer. The capability of Ta2O5-PAA to provide anatomical contrast-enhancing features has been demonstrated via computed tomography. The Ta2O5-PAA conjugate was further loaded with methotrexate, and the drug release was observed for a total of 72 h at a pH of 3.6, 5.4, 7.4, and 9.4. While the different layer thicknesses did not influence the drug release kinetics, a decrease in pH of the release medium resulted in a slower drug release. The developed nanocomposite particles present a great potential as a theranostic system for biomedical applications.


Assuntos
Resinas Acrílicas/química , Antimetabólitos Antineoplásicos/química , Metotrexato/química , Nanopartículas/química , Óxidos/química , Tantálio/química , Liberação Controlada de Fármacos , Concentração de Íons de Hidrogênio , Cinética , Estrutura Molecular , Tamanho da Partícula , Propriedades de Superfície , Difração de Raios X
4.
Nat Commun ; 6: 8689, 2015 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-26507613

RESUMO

Sodium-metal sulfide battery holds great promise for sustainable and cost-effective applications. Nevertheless, achieving high capacity and cycling stability remains a great challenge. Here, uniform yolk-shell iron sulfide-carbon nanospheres have been synthesized as cathode materials for the emerging sodium sulfide battery to achieve remarkable capacity of ∼ 545 mA h g(-1) over 100 cycles at 0.2 C (100 mA g(-1)), delivering ultrahigh energy density of ∼ 438 Wh kg(-1). The proven conversion reaction between sodium and iron sulfide results in high capacity but severe volume changes. Nanostructural design, including of nanosized iron sulfide yolks (∼ 170 nm) with porous carbon shells (∼ 30 nm) and extra void space (∼ 20 nm) in between, has been used to achieve excellent cycling performance without sacrificing capacity. This sustainable sodium-iron sulfide battery is a promising candidate for stationary energy storage. Furthermore, this spatially confined sulfuration strategy offers a general method for other yolk-shell metal sulfide-carbon composites.

5.
ACS Nano ; 8(10): 10920-30, 2014 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-25290080

RESUMO

Although much progress has been made to develop high-performance lithium-sulfur batteries (LSBs), the reported physical or chemical routes to sulfur cathode materials are often multistep/complex and even involve environmentally hazardous reagents, and hence are infeasible for mass production. Here, we report a simple ball-milling technique to combine both the physical and chemical routes into a one-step process for low-cost, scalable, and eco-friendly production of graphene nanoplatelets (GnPs) edge-functionalized with sulfur (S-GnPs) as highly efficient LSB cathode materials of practical significance. LSBs based on the S-GnP cathode materials, produced by ball-milling 70 wt % sulfur and 30 wt % graphite, delivered a high initial reversible capacity of 1265.3 mAh g(-1) at 0.1 C in the voltage range of 1.5-3.0 V with an excellent rate capability, followed by a high reversible capacity of 966.1 mAh g(-1) at 2 C with a low capacity decay rate of 0.099% per cycle over 500 cycles, outperformed the current state-of-the-art cathode materials for LSBs. The observed excellent electrochemical performance can be attributed to a 3D "sandwich-like" structure of S-GnPs with an enhanced ionic conductivity and lithium insertion/extraction capacity during the discharge-charge process. Furthermore, a low-cost porous carbon paper pyrolyzed from common filter paper was inserted between the 0.7S-0.3GnP electrode and porous polypropylene film separator to reduce/eliminate the dissolution of physically adsorbed polysulfide into the electrolyte and subsequent cross-deposition on the anode, leading to further improved capacity and cycling stability.

6.
ACS Appl Mater Interfaces ; 6(19): 16679-86, 2014 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-25198621

RESUMO

The significance of developing implantable, biocompatible, miniature power sources operated in a low current range has become manifest in recent years to meet the demands of the fast-growing market for biomedical microdevices. In this work, we focus on developing high-performance cathode material for biocompatible zinc/polymer batteries utilizing biofluids as electrolyte. Conductive polymers and graphene are generally considered to be biocompatible and suitable for bioengineering applications. To harness the high electrical conductivity of graphene and the redox capability of polypyrrole (PPy), a polypyrrole fiber/graphene composite has been synthesized via a simple one-step route. This composite is highly conductive (141 S cm(-1)) and has a large specific surface area (561 m(2) g(-1)). It performs more effectively as the cathode material than pure polypyrrole fibers. The battery constructed with PPy fiber/reduced graphene oxide cathode and Zn anode delivered an energy density of 264 mWh g(-1) in 0.1 M phosphate-buffer saline.


Assuntos
Materiais Biocompatíveis/química , Fontes de Energia Elétrica , Grafite/química , Nanofibras/química , Nanotecnologia/métodos , Polímeros/química , Pirróis/química , Zinco/química , Espectroscopia Dielétrica , Condutividade Elétrica , Técnicas Eletroquímicas , Eletrodos , Íons/sangue , Nanofibras/ultraestrutura , Espectroscopia Fotoeletrônica , Análise Espectral Raman
7.
Sci Rep ; 4: 6095, 2014 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-25168783

RESUMO

Nano-Germanium/polypyrrole composite has been synthesized by chemical reduction method in aqueous solution. The Ge nanoparticles were directly coated on the surface of the polypyrrole. The morphology and structural properties of samples were determined by X-ray diffraction, scanning electron microscopy and transmission electron microscopy. Thermogravimetric analysis was carried out to determine the polypyrrole content. The electrochemical properties of the samples have been investigated and their suitability as anode materials for the lithium-ion battery was examined. The discharge capacity of the Ge nanoparticles calculated in the Ge-polypyrrole composite is 1014 mAh g(-1) after 50 cycles at 0.2 C rate, which is much higher than that of pristine germanium (439 mAh g(-1)). The composite also demonstrates high specific discharge capacities at different current rates (1318, 1032, 661, and 460 mAh g(-1) at 0.5, 1.0, 2.0, and 4.0 C, respectively). The superior electrochemical performance of Ge-polypyrrole composite could be attributed to the polypyrrole core, which provides an efficient transport pathway for electrons. SEM images of the electrodes have demonstrated that polypyrrole can also act as a conductive binder and alleviate the pulverization of electrode caused by the huge volume changes of the nanosized germanium particles during Li(+) intercalation/de-intercalation.

8.
Dalton Trans ; 40(48): 12801-7, 2011 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-21637877

RESUMO

A tin nanoparticle/polypyrrole (nano-Sn/PPy) composite was prepared by chemically reducing and coating Sn nanoparticles onto the PPy surface. The composite shows a much higher surface area than the pure nano-Sn reference sample, due to the porous higher surface area of PPy and the much smaller size of Sn in the nano-Sn/PPy composite than in the pure tin nanoparticle sample. Poly(vinylidene fluoride) (PVDF) and sodium carboxymethyl cellulose (CMC) were also used as binders, and the electrochemical performance was investigated. The electrochemical results show that both the capacity retention and the rate capability are in the same order of nano-Sn/PPy-CMC > nano-Sn/PPy-PVDF > nano-Sn-CMC > nano-Sn-PVDF. Scanning electronic microscopy (SEM) and electrochemical impedance spectroscopy (EIS) results show that CMC can prevent the formation of cracks in electrodes caused by the big volume changes during the charge-discharge process, and the PPy in the composite can provide a conducting matrix and alleviate the agglomeration of Sn nanoparticles. The present results indicate that the nano-Sn/PPy composite could be suitable for the next generation of anode materials with relatively good capacity retention and rate capability.

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