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1.
RSC Adv ; 14(24): 16661-16677, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38784421

RESUMEN

This study explores the iodine and nickel-doped cobalt hydroxide (I & Ni-co-doped-Co(OH)2) as a potential material for energy storage and conversion applications owing to its excellent electrochemical characteristics. According to our analysis, it was revealed that this material exhibits pseudocapacitive-like behavior, as evident from distinct redox peaks observed in cyclic voltammetry, which confirms its ability to store charges. The diffusion coefficient analysis reveals that this material possesses conductivity and rapid diffusion kinetics, making it particularly advantageous compared to materials synthesized in previous studies. Charge-discharge measurements were performed to analyze the charge storage capacity and stability of this material after 3000 consecutive cycles, showing its excellent stability with minimum loss of capacitance. Furthermore, its anodic and cathodic linear sweep voltammetry curves were measured to evaluate its oxygen evolution and hydrogen evolution reaction performance. The results showed that the material exhibited an excellent water splitting performance, which suggests its potential practical application for hydrogen production. This increased activity was attributed to the doping of α-Co(OH)2, which improved its structural stability, electrical conductivity, and charge transfer efficiency. Thus, I & Ni-co-doped-Co(OH)2 possesses enhanced properties that make it an excellent material for both energy storage and hydrogen generation applications.

2.
Dalton Trans ; 53(19): 8177-8190, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38683625

RESUMEN

Exploring new strategies to design non-precious and efficient electrocatalysts can provide a solution for sluggish electrocatalytic kinetics and sustainable hydrogen energy. Transition metal selenides are potential contenders for bifunctional electrocatalysis owing to their unique layered structure, low band gap, and high intrinsic activities. However, insufficient access to active sites, lethargic water dissociation, and structural degradation of active materials during electrochemical reactions limit their activities, especially in alkaline media. In this article, we report a useful strategy to assemble vanadium diselenide (VSe2) into a 3D MXene/rGO-based sponge-like architecture (VSe2@G/MXe) using hydrothermal and freeze-drying approaches. The 3D hierarchical meso/macro-pore rich sponge-like morphology not only prevents aggregation of VSe2 nanosheets but also offers a kinetics-favorable framework and high robustness to the electrocatalyst. Synergistic coupling of VSe2 and a MXene/rGO matrix yields a heterostructure with a large specific surface area, high conductivity, and multi-dimensional anisotropic pore channels for uninterrupted mass transport and gas diffusion. Consequently, VSe2@G/MXe presented superior electrochemical activity for both the HER and OER compared to its counterparts (VSe2 and VSe2@G), in alkaline media. The overpotentials required to reach a cathodic and anodic current density of 10 mA cm-2 were 153 mV (Tafel slope = 84 mV dec-1) and 241 mV (Tafel slope = 87 mV dec-1), respectively. The Rct values at the open circuit voltage were as low as 9.1 Ω and 1.41 Ω for the HER and OER activity, respectively. Importantly, VSe2@G/MXe withstands a steady current output for a long 24 h operating time. Hence, this work presents a rational design for 3D microstructures with optimum characteristics for efficient bifunctional alkaline water-splitting.

3.
RSC Adv ; 13(43): 29944-29958, 2023 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-37842667

RESUMEN

The rapid recombination of charges of photogenerated electrons and holes severely limits single semiconductor photocatalytic applications. In this study, a simple and facile sol-gel approach was used to synthesize Ba2-xHoxSr2-yNiyFe12O22 (x = 0, 0.1 and y = 0, 0.5). The composite of holmium-nickel doped barium-strontium ferrite with MXene (Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene) was synthesized by ultrasonication method. These synthesized samples were subsequently used to photodegrade rhodamine B (RhB) and pendimethalin under visible light illumination. The results of the experiments demonstrated that MXene, as a cocatalyst, considerably reduces the rate of recombination of charges and broadens absorption of visible light by providing increased surface functional groups to improve the photocatalytic activity of synthesized samples. MXene is thermally stable, have high electrical conductivity, have adjustable bandgap, and hydrophilic in nature. The optimized Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene composite demonstrated an excellent photocatalytic rate by degrading 78.88% RhB and 75.59% pendimethalin in 140 minutes. Moreover, the scavenging experiment revealed that photogenerated electrons and holes were the primary active species involved in RhB and pendimethalin photodegradation, respectively. Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene showed increased photocatalytic behavior because it has increased surface area which decreases rate of recombination of electron and hole pair, hence photocatalytic activity increases. It is observed that Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene has potential application in photocatalytic degradation of harmful pollutants.

4.
Angew Chem Int Ed Engl ; 61(18): e202202087, 2022 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-35212442

RESUMEN

Electrocatalytic NO reduction is regarded as an attractive strategy to degrade the NO contaminant into useful NH3 , but the lack of efficient and stable electrocatalysts to facilitate such multiple proton-coupled electron-transfer processes impedes its applications. Here, we report on developing amorphous B2.6 C supported on a TiO2 nanoarray on a Ti plate (a-B2.6 C@TiO2 /Ti) as an NH3 -producing nanocatalyst with appreciable activity and durability toward the NO electroreduction. It shows a yield of 3678.6 µg h-1 cm-2 and a FE of 87.6 %, superior to TiO2 /Ti (563.5 µg h-1 cm-2 , 42.6 %) and a-B2.6 C/Ti (2499.2 µg h-1 cm-2 , 85.6 %). An a-B2.6 C@TiO2 /Ti-based Zn-NO battery achieves a power density of 1.7 mW cm-2 with an NH3 yield of 1125 µg h-1 cm-2 . An in-depth understanding of catalytic mechanisms is gained by theoretical calculations.

5.
Nanomaterials (Basel) ; 12(4)2022 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-35215041

RESUMEN

Tungsten oxide (WO3), MXene, and an WO3/MXene nanocomposite were synthesized to study their photocatalytic and biological applications. Tungsten oxide was synthesized by an easy and cost-effective hydrothermal method, and its composite with MXene was prepared through the sonication method. The synthesized tungsten oxide, MXene, and its composite were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Fourier transform infrared (FTIR), energy-dispersive X-ray analysis (EDX), and Brunauer-Emmett-Teller (BET) for their structural, morphological, spectral, elemental and surface area analysis, respectively. The crystallite size of WO3 calculated from XRD was ~10 nm, the particle size of WO3 was 130 nm, and the average thickness of MXene layers was 175 nm, which was calculated from FESEM. The photocatalytic activity of as-synthesized samples was carried out for the degradation of methylene blue under solar radiation, MXene, the WO3/MXene composite, and WO3 exhibited 54%, 89%, and 99% photocatalytic degradation, respectively. WO3 showed maximal degradation ability; by adding WO3 to MXene, the degradation ability of MXene was enhanced. Studies on antibacterial activity demonstrated that these samples are good antibacterial agents against positive strains, and their antibacterial activity against negative strains depends upon their concentration. Against positive strains, the WO3/MXene composite's inhibition zone was at 7 mm, while it became 9 mm upon increasing the concentration. This study proves that WO3, MXene, and the WO3/MXene nanocomposite could be used in biological and environmental applications.

6.
Small ; 18(13): e2106961, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35146914

RESUMEN

NiCo2 O4 nanowire array on carbon cloth (NiCo2 O4 /CC) is proposed as a highly active electrocatalyst for ambient nitrate (NO3 - ) reduction to ammonia (NH3 ). In 0.1 m NaOH solution with 0.1 m NaNO3 , such NiCo2 O4 /CC achieves a high Faradic efficiency of 99.0% and a large NH3 yield up to 973.2 µmol h-1  cm-2 . The superior catalytic activity of NiCo2 O4 comes from its half-metal feature and optimized adsorption energy due to the existence of Ni in the crystal structure. A Zn-NO3 - battery with NiCo2 O4 /CC cathode also shows a record-high battery performance.

7.
Adv Sci (Weinh) ; 9(8): e2103814, 2022 03.
Artículo en Inglés | MEDLINE | ID: mdl-35084113

RESUMEN

Since the discovery of single-layer graphene in 2004, the family of 2D inorganic nanosheets is considered as ideal membrane materials due to their ultrathin atomic thickness and fascinating physicochemical properties. However, the intrinsically nonporous feature of 2D inorganic nanosheets hinders their potential to achieve a higher flux to some extent. Recently, 2D polymer nanosheets, originated from the regular and periodic covalent connection of the building units in 2D plane, have emerged as promising candidates for preparing ultrafast and highly selective membranes owing to their inherently tunable and ordered pore structure, light weight, and high specific surface. In this review, the synthetic methodologies (including top-down and bottom-up methods) of 2D polymer nanosheets are first introduced, followed by the summary of 2D polymer nanosheets-based membrane fabrication as well as membrane applications in the fields of gas separation, water purification, organic solvent separation, and ion exchange/transport in fuel cells and lithium-sulfur batteries. Finally, based on their current achievements, the authors' personal insights are put forward into the existing challenges and future research directions of 2D polymer nanosheets for membrane separation. The authors believe this comprehensive review on 2D polymer nanosheets-based membrane separation will definitely inspire more studies in this field.

8.
Adv Mater ; 33(25): e2004557, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-33984164

RESUMEN

2D layered materials typically feature strong in-plane covalent chemical bonding within each atomic layer and weak out-of-plane van der Waals (vdW) interactions between adjacent layers. The non-bonding nature between neighboring layers naturally results in a vdW gap, in which various foreign species may be inserted without breaking the in-plane covalent bonds. By tailoring the composition, size, structure, and electronic properties of the intercalated guest species and the hosting layered materials, an expansive family of layered intercalation materials may be produced with highly variable compositional and structural features as well as widely tunable physical/chemical properties, invoking unprecedented opportunities in fundamental studies of property modulation and potential applications in diverse technologies, including electronics, optics, superconductors, thermoelectrics, catalysis, and energy storage. Here, the principles and protocols for various intercalation methods, including wet chemical intercalation, gas-phase intercalation, electrochemical intercalation, and ion-exchange intercalation, are comprehensively reviewed and how the intercalated species alter the crystal structure and the interlayer coupling of the host 2D layered materials, introducing unusual physical and chemical properties and enabling devices with superior performance or unique functions, is discussed. To conclude, a brief summary on future research opportunities and emerging challenges in the layered intercalation materials is given.

9.
Nature ; 591(7850): 385-390, 2021 03.
Artículo en Inglés | MEDLINE | ID: mdl-33731947

RESUMEN

Two-dimensional (2D) materials1,2 and the associated van der Waals (vdW) heterostructures3-7 have provided great flexibility for integrating distinct atomic layers beyond the traditional limits of lattice-matching requirements, through layer-by-layer mechanical restacking or sequential synthesis. However, the 2D vdW heterostructures explored so far have been usually limited to relatively simple heterostructures with a small number of blocks8-18. The preparation of high-order vdW superlattices with larger number of alternating units is exponentially more difficult, owing to the limited yield and material damage associated with each sequential restacking or synthesis step8-29. Here we report a straightforward approach to realizing high-order vdW superlattices by rolling up vdW heterostructures. We show that a capillary-force-driven rolling-up process can be used to delaminate synthetic SnS2/WSe2 vdW heterostructures from the growth substrate and produce SnS2/WSe2 roll-ups with alternating monolayers of WSe2 and SnS2, thus forming high-order SnS2/WSe2 vdW superlattices. The formation of these superlattices modulates the electronic band structure and the dimensionality, resulting in a transition of the transport characteristics from semiconducting to metallic, from 2D to one-dimensional (1D), with an angle-dependent linear magnetoresistance. This strategy can be extended to create diverse 2D/2D vdW superlattices, more complex 2D/2D/2D vdW superlattices, and beyond-2D materials, including three-dimensional (3D) thin-film materials and 1D nanowires, to generate mixed-dimensional vdW superlattices, such as 3D/2D, 3D/2D/2D, 1D/2D and 1D/3D/2D vdW superlattices. This study demonstrates a general approach to producing high-order vdW superlattices with widely variable material compositions, dimensions, chirality and topology, and defines a rich material platform for both fundamental studies and technological applications.

10.
J Tissue Eng Regen Med ; 15(4): 322-335, 2021 04.
Artículo en Inglés | MEDLINE | ID: mdl-33432773

RESUMEN

The importance of bone scaffolds has increased many folds in the last few years; however, during bone implantation, bacterial infections compromise the implantation and tissue regeneration. This work is focused on this issue while not compromising on the properties of a scaffold for bone regeneration. Biocomposite scaffolds (BS) were fabricated via the freeze-drying technique. The samples were characterized for structural changes, surface morphology, porosity, and mechanical properties through spectroscopic (Fourier transform-infrared [FT-IR]), microscopic (scanning electron microscope [SEM]), X-ray (powder X-ray diffraction and energy-dispersive X-ray), and other analytical (Brunauer-Emmett-Teller, universal testing machine Instron) techniques. Antibacterial, cellular, and hemocompatibility assays were performed using standard protocols. FT-IR confirmed the interactions of all the components. SEM illustrated porous and interconnected porous morphology. The percentage porosity was in the range of 49.75%-67.28%, and the pore size was 215.65-470.87 µm. The pore size was perfect for cellular penetration. Thus, cells showed significant proliferation onto these scaffolds. X-ray studies confirmed the presence of nanohydroxyapatite and graphene oxide (GO). The cell viability was 85%-98% (BS1-BS3), which shows no significant toxicity of the biocomposite. Furthermore, the biocomposites exhibited better antibacterial activity, no effect on the blood clotting (normal in vitro blood clotting), and less than 5% hemolysis. The ultimate compression strength for the biocomposites increased from 4.05 to 7.94 with an increase in the GO content. These exciting results revealed that this material has the potential for possible application in bone tissue engineering.


Asunto(s)
Durapatita/química , Curación de Fractura , Fracturas Óseas/patología , Grafito/química , Nanopartículas/química , Alcohol Polivinílico/química , Andamios del Tejido/química , Xilanos/química , Animales , Antibacterianos/farmacología , Coagulación Sanguínea/efectos de los fármacos , Adhesión Celular/efectos de los fármacos , Muerte Celular/efectos de los fármacos , Forma de la Célula/efectos de los fármacos , Supervivencia Celular/efectos de los fármacos , Curación de Fractura/efectos de los fármacos , Pruebas de Sensibilidad Microbiana , Porosidad , Ratas , Espectrometría por Rayos X , Espectroscopía Infrarroja por Transformada de Fourier , Agua , Difracción de Rayos X
11.
J Hazard Mater ; 402: 123526, 2021 01 15.
Artículo en Inglés | MEDLINE | ID: mdl-32758998

RESUMEN

An efficient, environment-friendly and economical catalyst to control contaminants of environment is an enduring interest in recent years. In this study, a new composite, DyxMnFe2-xO4nanoparticles decorated over mesoporous silica was synthesized and utilized for removal of organic pollutant. Highly crystalline nature of DyxMnFe2-xO4 nanoparticles and amorphous nature of material was confirmed by XRD (X-ray diffraction) technique. Infrared spectra of fabricated material before and after adsorption of dye molecules evidenced the successful adsorption of dye molecules by fabricated adsorbent. From field emission scanning electron microscopic (FESEM) images of Dy3+ substituted MnFe2O4 composite with mesoporous silica, it was clearly observed that ferrite particles of size 20-30 nm were decorated on the surface of mesoporous silica particles and distributed well over spherical silica balls homogeneously. Its magnificent mesoporous nature was revealed from BET (nitrogen adsorption-desorption measurements) analysis. Surface area, pore volume and average pore size was found 387.95 m2/g, 0.390 cm3/g and 4.02 nm respectively. Tri-modal pore size distribution showed its effective utilization in adsorption. The abundant (SiOH) hydroxyl groups of mesoporous silica, the broad diffraction hump of silica depicted its superior loading capacity of target molecular specie inside its porous network. From band gap analysis, a red shift of 2.43 eV exhibited semiconductor photocatalysis of DyxMnFe2-xO4 nanoparticles. Degradation efficiency of bare MnFe2O4, DyxMnFe2-xO4 and mesoporous silica-based composite was tested using crystal violet dye. Its explored adsorption-photocatalysis synergy, degradation mechanism, kinetic investigation, easily recovery and remarkable recycling ability suggested that the new fabricated composite is best for environmental remediation.

12.
ACS Omega ; 5(41): 26845-26854, 2020 Oct 20.
Artículo en Inglés | MEDLINE | ID: mdl-33111010

RESUMEN

Recently, a new class of two-dimensional (2D) materials, called MXene, consisting of layers of transition-metal carbides and nitrides/carbonitrides has been introduced. MXene, a multifunctional material with hydrophilic nature and excellent electrical conductivity and chemical stabilities, can be applied in diverse research areas such as energy harvesting and its storage, water purification, thermal dissipation, and gas sensing. To achieve the best quality of MXene, optimization of some important synthetic parameters is highly required such as an optimized etchant concentration to remove an "A" element from the MAX phase and sonication time for the efficient exfoliation of MXene flakes. Besides, there is a need to disclose that particular solvent through which intercalation can easily be achieved. In this work, we optimized the abovementioned critical parameters for the synthesis of good-quality MXene. Our results clearly explain the variations in the quality of MXene under applied etchant concentrations, solvents for better intercalation, and optimization of sonication time for better exfoliation. The obtained results suggest that 30% HF as an etchant, dimethyl sulfoxide (DMSO) as a solvent, and 135 min as the sonication time are effective parameters for the synthesis of good-quality MXene. We expect that this report will be helpful for the young research community to synthesize good-quality MXene with the required properties.

13.
J Tissue Eng Regen Med ; 14(10): 1488-1501, 2020 10.
Artículo en Inglés | MEDLINE | ID: mdl-32761978

RESUMEN

It is a challenging task to develop active biomacromolecular wound dressing materials that are biocompatible and possesses antibacterial properties against the bacterial strains that cause severe skin disease. This work is focused on the preparation of a biocompatible and degradable hydrogel for wound dressing application using arabinoxylan (ARX) and guar gum (GG) natural polymers. Fourier transform infrared spectroscopy (FT-IR) confirmed that both ARX and GG interacted well with each other, and their interactions further increased with the addition of crosslinker tetraethyl orthosilicate. Scanning electron microscope (SEM) micrographs showed uniform porous morphologies of the hydrogels. The porous morphologies and uniform interconnected pores are attributed to the increased crosslinking of the hydrogel. Elastic modulus, tensile strength, and fracture strain of the hydrogels significantly improved (from ATG-1 to ATG-4) with crosslinking. Degradability tests showed that hydrogels lost maximum weight in 7 days. All the samples showed variation in swelling with pH. Maximum swelling was observed at pH 7. The hydrogel samples showed good antibacterial activity against Pseudomonas aeruginosa (Gram-negative) and Staphylococcus aureus (Gram-positive) in PBS, good drug release profile (92% drug release), and nontoxic cellular behavior. The cells not only retained their cylindrical morphologies onto the hydrogel but were also performing their normal activities. It is, therefore, believed that as-developed hydrogel could be a potential material for wound dressing application.


Asunto(s)
Antiinfecciosos/farmacología , Vendajes , Materiales Biocompatibles/farmacología , Galactanos/farmacología , Hidrogeles/farmacología , Mananos/farmacología , Gomas de Plantas/farmacología , Piel/patología , Heridas y Lesiones/patología , Xilanos/farmacología , Animales , Línea Celular , Forma de la Célula/efectos de los fármacos , Liberación de Fármacos , Galactanos/química , Hidrogeles/química , Mananos/química , Ensayo de Materiales , Ratones , Pruebas de Sensibilidad Microbiana , Gomas de Plantas/química , Polímeros/química , Pseudomonas aeruginosa/efectos de los fármacos , Piel/efectos de los fármacos , Espectroscopía Infrarroja por Transformada de Fourier , Staphylococcus aureus/efectos de los fármacos , Resistencia a la Tracción , Xilanos/química
14.
Nat Nanotechnol ; 15(9): 768-775, 2020 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-32661372

RESUMEN

Lead halide perovskites have attracted increasing interest for their exciting potential in diverse optoelectronic devices. However, their charge transport properties remain elusive, plagued by the issues of excessive contact resistance and large hysteresis in ambient conditions. Here we report a van der Waals integration approach for creating high-performance contacts on monocrystalline halide perovskite thin films with minimum interfacial damage and an atomically clean interface. Compared to the deposited contacts, our van der Waals contacts exhibit two to three orders of magnitude lower contact resistance, enabling systematic transport studies in a wide temperature range. We report a Hall mobility exceeding 2,000 cm2 V-1 s-1 at around 80 K, an ultralow bimolecular recombination coefficient of 3.5 × 10-15 cm3 s-1 and a photocurrent gain >106 in the perovskite thin films. Furthermore, magnetotransport studies reveal a quantum-interference-induced weak localization behaviour with a phase coherence length up to 49 nm at 3.5 K. Our results lay the foundation for exploring new physics in this class of 'soft-lattice' materials.

15.
J Hazard Mater ; 394: 122593, 2020 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-32251904

RESUMEN

In the current investigation, graphene (rGO)-supported cerium substituted nickel ferrite (NiCeyFe2-yO4 y = 0.05) photocatalyst was prepared via two-step wet chemical approach. The resulting NiCeyFe2-yO4/rGO nanocomposite exhibited excellent photocatalytic performance and stability. Moreover, the photocatalytic activity of NiCeyFe2-yO4/rGO nanocomposite was also investigated comparatively with NiCeyFe2-yO4 nanoparticles. As compared to the NiCeyFe2-yO4 nanoparticles, NiCeyFe2-yO4/rGO nanocomposite showed superior photocatalytic efficiency and recycling stability for MB degradation, which is two times that of bare NiCeyFe2-yO4 nanoparticles. After visible light irradiation for 70 min, 94.67 % of MB dye was removed by NiCeyFe2-yO4/rGO nanocomposite whereas only 50 % of MB dye was removed by NiCeyFe2-yO4 nanoparticles. The increase in photocatalytic performance is mainly ascribed to formation of NiCeyFe2-yO4/rGO heterojunction which not only assist in separation of photo-induced charge carriers, but also sustain a strong redox ability. Moreover, the photo-corrosion of NiCe0.05Fe1.95O4 nanoparticles is inhibited through transfer of photo-induced electrons of NiCe0.05Fe1.95O4 nanoparticles to rGO. A possible photo-degradation mechanism based on reactive species trapping experiments has been proposed. The effect of various factors like pH, temperature and catalyst dosage has also been explored. Facile synthesis method, excellent photocatalytic performance for organic pollutants and superior reusability suggest that NiCeyFe2-yO4/rGO photocatalyst possesses high potential for large-scale pollutant treatment.

16.
Angew Chem Int Ed Engl ; 59(21): 8247-8254, 2020 May 18.
Artículo en Inglés | MEDLINE | ID: mdl-32049418

RESUMEN

A facile and versatile microwave-assisted and shell-confined Kirkendall diffusion strategy is used to fabricate ultrasmall hollow nanoparticles by modulating the growth and thermal conversion of metal-organic framework (MOF) nanocrystals on graphene. This method involves that the adsorption of microwave by graphene creates a high-energy environment in a short time to decompose the in situ grown MOF nanocrystals into well-dispersed uniform core-shell nanoparticles with ultrasmall size. Upon a shell-confined Kirkendall diffusion process, hollow nanoparticles of multi-metal oxides, phosphides, and sulfides with the diameter below 20 nm and shell thickness below 3 nm can be obtained for the first time. Ultrasmall hollow nanostructures such as Fe2O3 can promote much faster charge transport and expose more active sites as well as migrate the volume change stress more efficiently than the solid and large hollow counterparts, thus demonstrating remarkable lithium-ion storage performance.

17.
Chem Soc Rev ; 48(20): 5207-5241, 2019 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-31573024

RESUMEN

Electrocatalysis plays an essential role in diverse electrochemical energy conversion processes that are vital for improving energy utilization efficiency and mitigating the aggravating global warming challenge. The noble metals such as platinum are generally the most frequently used electrocatalysts to drive these reactions and facilitate the relevant energy conversion processes. The high cost and scarcity of these materials pose a serious challenge for the wide-spread adoption and the sustainability of these technologies in the long run, which have motivated considerable efforts in searching for alternative electrocatalysts with reduced loading of precious metals or based entirely on earth-abundant metals. Of particular interest are graphene-supported single atom catalysts (G-SACs) that integrate the merits of heterogeneous catalysts and homogeneous catalysts, such as high activity, selectivity, stability, maximized atom utilization efficiency and easy separation from reactants/products. The graphene support features a large surface area, high conductivity and excellent (electro)-chemical stability, making it a highly attractive substrate for supporting single atom electrocatalysts for various electrochemical energy conversion processes. In this review, we highlight the recent advancements in G-SACs for electrochemical energy conversion, from the synthetic strategies and identification of the atomistic structure to electrocatalytic applications in a variety of reactions, and finally conclude with a brief prospect on future challenges and opportunities.

18.
Science ; 363(6428): 723-727, 2019 02 15.
Artículo en Inglés | MEDLINE | ID: mdl-30765563

RESUMEN

Ceramic aerogels are attractive for thermal insulation but plagued by poor mechanical stability and degradation under thermal shock. In this study, we designed and synthesized hyperbolic architectured ceramic aerogels with nanolayered double-pane walls with a negative Poisson's ratio (-0.25) and a negative linear thermal expansion coefficient (-1.8 × 10-6 per °C). Our aerogels display robust mechanical and thermal stability and feature ultralow densities down to ~0.1 milligram per cubic centimeter, superelasticity up to 95%, and near-zero strength loss after sharp thermal shocks (275°C per second) or intense thermal stress at 1400°C, as well as ultralow thermal conductivity in vacuum [~2.4 milliwatts per meter-kelvin (mW/m·K)] and in air (~20 mW/m·K). This robust material system is ideal for thermal superinsulation under extreme conditions, such as those encountered by spacecraft.

19.
ACS Appl Mater Interfaces ; 11(2): 2218-2224, 2019 Jan 16.
Artículo en Inglés | MEDLINE | ID: mdl-30582695

RESUMEN

Graphene oxide (GO) is not only a unique class of two-dimensional (2D) materials but also an important precursor for scalable preparation of graphene. The efficient size fractionation of GO is of great importance to the fundamental and applied studies of chemically modified graphene, but remains a great challenge. Herein, we report an efficient and scalable fractionation method of GO employing reversible adsorption/desorption of temperature-responsive poly( N-isopropylacrylamide) on GO to amplify its mass difference and significantly improve the fractionation efficiency. Furthermore, size-dependent sodium ion storage of the resulting fractionated reduced GO (RGO) is revealed for the first time with high sodium storage performance achieved for the smallest RGO because of its largest d-spacing and most defect sites. This work provides valuable insights into the size fractionation and size-dependent electrochemical performance of graphene, which can be potentially extended to other 2D materials.

20.
ACS Nano ; 12(12): 12879-12887, 2018 Dec 26.
Artículo en Inglés | MEDLINE | ID: mdl-30525431

RESUMEN

Deliberate design of advantageous nanostructures holds great promise for developing high-performance electrode materials for electrochemical energy storage. However, it remains a tremendous challenge to simultaneously gain high gravimetric, areal, and volumetric capacities as well as high rate performance and cyclability to meet practical requirements mainly due to the intractable insufficient ion diffusion and limited active sites for dense electrodes with high areal mass loadings. Herein we report a double-holey-heterostructure framework, in which holey Fe2O3 nanosheets (H-Fe2O3) are tightly and conformably grown on the holey reduced graphene oxide (H-RGO). This hierarchical nanostructure allows for rapid ion and electron transport and sufficient utilization of active sites throughout a highly compact and thick electrode. Therefore, the free-standing flexible H-Fe2O3/H-RGO heterostructure anode can simultaneously deliver ultrahigh gravimetric, areal, and volumetric capacities of 1524 mAh g-1, 4.72 mAh cm-2, and 2621 mAh cm-3, respectively, at 0.2 A g-1 after 120 cycles, and extraordinary rate performance with a capacity of 487 mAh g-1 (1.51 mAh cm-2) at a high current density of 30 A g-1 (93 mA cm-2) as well as excellent cycling stability with a capacity retention of 96.3% after 1600 cycles, which has rarely been achieved before.

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