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1.
ACS Appl Mater Interfaces ; 16(32): 41996-42006, 2024 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-39079084

RESUMO

Vanadium tetrasulfide (VS4) is one of the most promising cathodic materials for rechargeable magnesium battery systems (RMBSs). Elemental substitution to expand layers, creation of sulfur vacancies, and reduction of particle sizes of VS4 are undoubtedly effective strategies to enhance cathodic performances. Experimental and DFT analysis revealed that valence states of vanadium and cobalt have been elevated from V2+ to V3+ and Co2+ to Co3+ in VS4 and that the Co-S bond length shortened due to cobalt substitution, which resulted in enhanced overall internal polarization in the layered atomic structure of VS4 by increasing cobalt concentrations. This phenomenon of charge accumulation contributes toward regulated magnesiation and accommodated volume expansion while cycling, resulting in the enormous structural stability of VS4 and sustainable battery performance during a long and stable cycling at a cost of 20% capacity diminution as compared to pristine VS4 in RMBS. Hence, 9% CoVS4 demonstrated a capacity of 158 mAh g-1 at a current density of 500 mA g-1 with approximately 98% capacity retention after 1000 cycles. Sustainable cathodic performance is the most desirous feature for commercialization. This work provides insight realization regarding structural limitations and opportunities of VS4 for sustainable cathodic performances in RMBS with non-nucleophilic 0.25 mol/L (R-PhOMgCI)2-A1Cl3/THF (PMC) electrolyte and has laid a theoretical plus experimental foundation for future developments.

2.
Small ; 20(27): e2309901, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38299768

RESUMO

Metal sulfides are promising anode materials for sodium-ion batteries (SIBs) due to their structural diversity and high theoretical capacity, but the severe capacity decay and inferior rate capability caused by poor structural stability and sluggish kinetics impede their practical applications. Herein, a cobalt-doped amorphous VS4 wrapped by reduced graphene oxide (i.e., Co0.5-VS4/rGO) is developed through a Co-induced defect engineering strategy to boost the kinetics performances. The as-prepared Co0.5-VS4/rGO demonstrates excellent rate capacities over 10 A g-1 and superior cycling stability at 5 A g-1 over 1600 cycles, which is attributed to the defects formed by Co doping, the formed amorphous structure and the robust rGO substrate. The great features of Co0.5-VS4/rGO anode are further confirmed in sodium-ion capacitors when the active carbon cathode is used. Additionally, the relationships between metal doping, the derived defects, the amorphous structure, and the sodium storage of VS4 are uncovered. This work provides deep insights into preparing amorphous functional materials and also probes the potential applications of metal sulfide-based electrode materials for advanced batteries.

3.
J Colloid Interface Sci ; 660: 907-915, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38280283

RESUMO

Development of high-performance metal sulfides anode materials is a great challenge for sodium-ion batteries (SIBs). In this work, a cobalt-based imidazolate framework (ZIF-67) were firstly synthesized and applied as precursor. After the successive surface etching, ion exchange and sulfidation processes, the final cobalt-vanadium sulfide yolk-shell nanocages were obtained (CoS2/VS4@NC) with VS4 shell and CoS2 yolk encapsulated into nitrogen doped carbon frameworks. This yolk-shell nanocage structure effectively increases the specific surface area and provides enough space for inhibiting the volume change during charge/discharge processes. Besides, the nitrogen doped carbon skeleton greatly improves the ionic conductivity and facilitates ion transport. When used as the anode materials for SIBs, the yolk-shell nanocages of CoS2/VS4@NC electrode exhibits excellent rate capability and stable cycle performance. Notably, it displays a long-term cycling stability with excellent capacity of 417.28 mA h g-1 after 700 cycles at a high current density of 5 A/g. This developed approach here provides a new route for the design and synthesis of various yolk-shell nanocages nanomaterials from enormous MOFs with multitudinous compositions and morphologies and can be extended to the application into other secondary batteries and energy storage fields.

4.
ACS Appl Mater Interfaces ; 15(31): 37442-37453, 2023 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-37494549

RESUMO

V-based sulfides are considered as potential cathode materials for Mg2+/Li+ hybrid ion batteries (MLIBs) due to their high theoretical specific capacities, unique crystal structure, and flexible valence adjustability. However, the formation of irreversible polysulfides, poor cycling performance, and severe structural collapse at high current densities impede their further development. Herein, VS4 microspheres with various controllable nanoarchitectures were successfully constructed via a facile solvothermal method by adjusting the amount of hydrochloric acid and were used as cathode materials for MLIBs. The VS4 microsphere self-assembled by bundles of paralleled-nanorods and some intersected-nanorods (VS4@NC-5) exhibits an outstanding initial discharge capacity of 805.4 mAh g-1 at 50 mA g-1 that is maintained at 259.1 mAh g-1 after 70 cycles. Moreover, the VS4@NC-5 cathode can deliver a superior rate capability (146.1 mAh g-1 at 2000 mA g-1) and ultralong cycling life (134.5 mAh g-1 at 2000 mA g-1 after 2000 cycles). The extraordinary electrochemical performance of VS4@NC-5 could be attributed to its special multi-hierarchical microsphere structure and the formation of N-doped carbon layers and V-C bonds, resulting in unobstructed ion diffusion channels, multidimensional electron transfer pathways, and enhancements of electrical conductivity and structure stability. Furthermore, the electrochemical reaction mechanism and phase conversion behavior of the VS4@NC-5 cathode at various states are investigated by a series of ex situ characterization methods. The VS4 well-designed through morphological engineering in this work can pave a way to explore more sulfides with high-rate performance and long cycling stability for energy storage devices.

5.
J Colloid Interface Sci ; 650(Pt A): 480-489, 2023 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-37421750

RESUMO

Lithium-sulfur (Li-S) batteries are regarded as highly prospective energy storage devices. However, problems such as low sulfur utilization, poor cycle performance, and insufficient rate capability hinder the commercial development of Li-S batteries. Three-dimensional (3D) structure materials have been applied to modify the separator of Li-S batteries to suppress the diffusion of lithium polysulfides (LiPSs) and inhibit the transmembrane diffusion of Li+. A vanadium sulfide/titanium carbide (VS4/Ti3C2Tx) MXene composite with a 3D conductive network structure has been synthesized in situ by a simple hydrothermal reaction. VS4 is uniformly loaded on the Ti3C2Tx nanosheets through vanadium-carbon(V-C) bonds, which effectively inhibits the self-stacking of Ti3C2Tx. The synergistic action of VS4 and Ti3C2Tx substantially reduces the shuttle of LiPSs, improves interfacial charge transfer, and boosts the kinetics of LiPSs conversion, consequently increasing the rate performance and cycle stability of the battery. The assembled battery has a specific discharge capacity of 657 mAhg-1 after 500 cycles at 1C, with a high capacity retention rate of 71%. The construction of VS4/Ti3C2Tx composite with a 3D conductive network structure provides a feasible strategy for the application of polar semiconductor materials in Li-S batteries. It also provides an effective solution for the design of high-performance Li-S batteries.

6.
J Colloid Interface Sci ; 649: 194-202, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37348339

RESUMO

Elaborate and rational design of cost-effective and high-efficiency non-noble metal electrocatalysts for pushing forward the sustainable hydrogen fuel production is of great significance. Herein, a novel VS4 nanoparticle decorated Ni3S2 nanobelt array in-situ grown on nickel foam (VS4/Ni3S2/NF NBs) was prepared by a self-templated synthesis strategy. Benefitting from the unique nanobelt array structure, abundant highly active bridge S22- sites and strong electronic interaction between VS4 and Ni3S2 on the heterointerface, the integrated VS4/Ni3S2/NF NBs exhibited excellent electrocatalytic hydrogen evolution activity and robust stability. The density functional theory (DFT) further revealed the reversible conversion catalysis mechanism of bridging S22- sites in VS4/Ni3S2/NF NBs during HER process. Notably, bidentate bridging SS bonds as the predominant catalytically active centers can spontaneously open once H adsorbed its surface, leading to the aggregation of negative charges on S atoms and thus facilitating the generation of H* intermediates, and spontaneously close when H* desorption is going to form H2. Our work provides fresh insights for developing potential polysulfides as high-performance hydrogen-evolving electrocatalysts for prospective clean energy production from water splitting.

7.
ACS Appl Mater Interfaces ; 15(5): 6888-6901, 2023 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-36696545

RESUMO

Rechargeable aluminum batteries (RABs) are gaining widespread attention for large-scale energy storage applications as a result of their high energy densities, high security, and abundance. The key to sustain the progress of RABs lies in the quest for the proper cathode materials with prominent capacity and reversible cycle life. Herein, we propose a tremella-like VS4 as a cathode material aiming to tackle this problem. Obtained from a morphology modification process, VS4 with a unique nanosheet structure provides sufficient active sites for intercalation and conversion reactions, shortens the transport paths for charge carrier ions, and facilitates the infiltration process for electrolyte. The RAB with the VS4 cathode exhibits excellent electrochemical performance, including outstanding specific capacity (407.9 mAh g-1) and stable cycling performance (∼300 cycles at a high current density). The energy storage mechanism has been comprehensively investigated and is confirmed to be a combination of the intercalation/deintercalation of Al3+ and AlCl4- ions and conversion reaction by various techniques and DFT calculation. Our study not only provides a peculiar and simple strategy for the rational design of metal sulfide cathode materials with high capacity and long-term stability but also proposes a specific energy storage mechanism that guides the development of cathode materials of RABs in the future.

8.
J Colloid Interface Sci ; 635: 358-369, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36599235

RESUMO

Transition metal sulfides have been demonstrated to be effective for peroxymonosulfate (PMS) activation towards wastewater treatment. However, the activity of vanadium sulfide (VS4) and the role of the chemical state of V have not been revealed. Here, three types of VS4 with various morphologies and chemical states of V were synthesized by using methanol (M-VS4, nanosphere composed of nanosheets), ethanol (E-VS4, sea urchin like nanosphere) and ultrapure water (U-VS4, compact nanosphere) as hydrothermal solvent, respectively, and used as heterogeneous catalysts to activate PMS for the degradation of refractory organic pollutants. The effects of PMS concentration, temperature, pH, inorganic ions, and humic acid (HA) on the degradation efficiency of VS4/PMS system were investigated systematically. The results indicated that the highest specific surface area and lowest ratio of V5+ enable E-VS4/PMS system possessed the highest performance in degrading tetracycline hydrochloride (TCH), in which 100% TCH was removed after operating 10 min (0.805 min-1) under a relatively low concentration of PMS (1 mM) and catalyst (100 mg/L). It also revealed that the system exhibited a typical radical process in TCH degradation, which could be attributed to the redox cycles between V5+, V4+ and V3+ in the presence of PMS to generate various radicals. This radical process enabled the E-VS4/PMS system with a high activity in wide reaction conditions and high mineralization ratios in degrading various refractory organic pollutants within 10 min. In addition, the E-VS4/PMS system exhibited favorable reusability and stability with very less V and S ions leaching, and showed excellent performance in real water purification.

9.
ACS Nano ; 16(8): 12900-12909, 2022 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-35913207

RESUMO

The weak van der Waals interactions of the one-dimensional (1D) chainlike VS4 crystal structure can enable fast charge-transfer kinetics in metal ion batteries, but its potential has been rarely exploited in depth. Herein, a thermodynamics-driven morphology manipulation strategy is reported to tailor VS4 nanosheets into 3D hierarchical self-assembled architectures including nanospheres, hollow nanospheres, and nanoflowers. The ultrathin VS4 nanosheets are generated via 2D anisotropic growth by the strong driving force of coordination interaction from ammonium ions under microwave irradiation and then evolve into 3D sheet-assembled configurations by adjusting the thermodynamic factors of temperature and reaction time. The as-synthesized VS4 nanomaterials present good electrochemical performances as the anode materials for sodium-ion batteries. In particular, the hollow VS4 nanospheres show a specific capacity of 1226.7 mAh g-1 at 200 mA g-1 current density after 100 cycles. The hierarchical nanostructures with large specific surface area and structural stability can overcome the difficulty of sodium ions embedding into the bulk material interior and provide more reactive materials at the same material mass loading compared with other morphologies. Both experiment and DFT calculations suggest that VS4 nanosheets reduce reaction kinetic impediment of sodium ion in battery operating. This work demonstrates a way of the morphological design of 2D VS4 nanosheets and application in sodium ion storage.

10.
J Colloid Interface Sci ; 625: 41-49, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35714407

RESUMO

Developing electrode materials with desirable electrochemical properties for sodium and potassium ion batteries remains a tremendous challenge. Herein, hetero-structured hybrids with VS4 nanodots decorated on CoS2/NC dodecahedron (CoS2/NC@VS4) have been successfully synthesized through employing a cobalt-based imidazolate framework (ZIF-67) as a template to prepare CoS2/NC inner core. Then VS4 nanodots was then grown on the surface of CoS2/NC by hydrothermal method to construct a heterostructure. This heterogeneous structure facilitates full contact with the electrolytes and shortens electrons and ions diffusion distance. Besides, the nitrogen-doped carbon framework derived from ZIF-67 promotes electron transport and gives a reliable shield to buffer the volume swelling during discharge and charge processes. Driving by the synergistic effect of bimetallic sulfides and the multiple valence states vanadium sulfide, CoS2/NC@VS4 exhibits outstanding rate capability and stable cycle performance as the anode for SIBs and PIBs, including a specific capacity of 307 mAh g-1 at the current density of 1.0 A g-1 after 700 cycles for SIBs and a capacity of 291.54 mAh g-1 at the current density of 1.0 A g-1 after 430 cycles in PIBs.

11.
ACS Appl Mater Interfaces ; 13(45): 54005-54017, 2021 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-34739752

RESUMO

The development of cathode materials with a high electric conductivity and a low polarization effect is crucial for enhancing the electrochemical properties of magnesium-ion batteries (MIBs). Herein, Mo doping and nitrogen-doped tubular graphene (N-TG) introduction are carried out for decorating VS4 (Mo-VS4/N-TG) via the one-step hydrothermal method as a freestanding cathode for MIBs. The results of characterizations and density functional theory (DFT) reveal that rich sulfur vacancies are induced by Mo doping, and N-TG as a high conductive skeleton material serves to disperse the active material and forms a tight connection, all of which collectively improved the electrical conductivity of electrode and increased the adsorption energy of Mg2+ (-6.341 eV). Furthermore, the fast reaction kinetics is also confirmed by the galvanostatic intermittent titration technique (GITT) and the pesudocapacitance-like contribution analysis. Benefiting from the synergistic effect of electrical conductivity enhancement and rich vacancy introduction, Mo-VS4/N-TG delivers a steady Mg2+ storage specific capacity of about 140 mAh g-1 at 50 mA g-1, outstanding cycle stability (80.6% capacity retention ratio after 1200 cycles under 500 mA g-1), and excellent rate capability (specific capacity reaches 77.1 mAh g-1 when the current density reaches 500 mA g-1). In addition, the reversible reaction process, intercalation mechanism, and structural stability during the Mg2+ insertion/extraction process are confirmed by a series of ex situ characterizations. This research provides a sustainable and scalable strategy to spur the development of MIBs.

12.
J Colloid Interface Sci ; 574: 312-323, 2020 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-32335482

RESUMO

Exploring electrode materials with excellent electrochemical performance is the key to the development of applications in energy storage and conversion. Herein, three-dimensional (3D) vanadium sulfide/carbon nanotubes/reduced graphene oxide (VS4/CNTs/rGO) composite is synthesized by a simple one-step hydrothermal method. VS4 short nanorods cover the both sides of the rGO sheets, and CNTs distribute at the edge of the composite to form a sandwich-like structure, which effectively prevents the accumulation of rGO. Due to the special 3D hierarchical structure, VS4/CNTs/rGO exhibits a large specific surface area and a rich pore structure, and the addition of CNTs and rGO also improves the electrochemical properties of VS4. At 1 A·g-1, VS4/CNTs/rGO exhibits a capacitance of 497 F·g-1 (1374.0 C·g-1) in the voltage range of -1.4 to 1.4 V, which is much higher than those binary materials including CNTs/rGO, VS4/CNTs and VS4/rGO. The VS4/CNTs/rGO symmetric supercapacitor (SSC) device shows a remarkable electrochemical performance in a large potential window up to 2.2 V. The capacitance of VS4/CNTs/rGO SSC device can reach 1003.5 mF·cm-2 (2207.6 mC·cm-2) at 0.5 mA·cm-2, and it exhibits an energy density of 6.75 Wh·m-2 (72.07 Wh·kg-1) at a power density of 1.38 W·m-2 (14.69 W·kg-1). The high capacitance and energy density of the VS4/CNTs/rGO composite in the high voltage interval make it as the potential energy storage material.

13.
Angew Chem Int Ed Engl ; 59(28): 11483-11490, 2020 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-32220137

RESUMO

The development of multivalent metal (such as Mg and Ca) based battery systems is hindered by lack of suitable cathode chemistry that shows reversible multi-electron redox reactions. Cationic redox centres in the classical cathodes can only afford stepwise single-electron transfer, which are not ideal for multivalent-ion storage. The charge imbalance during multivalent ion insertion might lead to an additional kinetic barrier for ion mobility. Therefore, multivalent battery cathodes only exhibit slope-like voltage profiles with insertion/extraction redox of less than one electron. Taking VS4 as a model material, reversible two-electron redox with cationic-anionic contributions is verified in both rechargeable Mg batteries (RMBs) and rechargeable Ca batteries (RCBs). The corresponding cells exhibit high capacities of >300 mAh g-1 at a current density of 100 mA g-1 in both RMBs and RCBs, resulting in a high energy density of >300 Wh kg-1 for RMBs and >500 Wh kg-1 for RCBs. Mechanistic studies reveal a unique redox activity mainly at anionic sulfides moieties and fast Mg2+ ion diffusion kinetics enabled by the soft structure and flexible electron configuration of VS4 .

14.
Nanomicro Lett ; 12(1): 39, 2020 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-34138251

RESUMO

Sodium-ion batteries (SIBs) are considered to be attractive candidates for large-scale energy storage systems because of their rich earth abundance and consistent performance. However, there are still challenges in developing desirable anode materials that can accommodate rapid and stable insertion/extraction of Na+ and can exhibit excellent electrochemical performance. Herein, the self-assembled hairball-like VS4 as anodes of SIBs exhibits high discharge capacity (660 and 589 mAh g-1 at 1 and 3 A g-1, respectively) and excellent rate property (about 100% retention at 10 and 20 A g-1 after 1000 cycles) at room temperature. Moreover, the VS4 can also exhibit 591 mAh g-1 at 1 A g-1 after 600 cycles at 0 °C. An unlike traditional mechanism of VS4 for Na+ storage was proposed according to the dates of ex situ characterization, cyclic voltammetry, and electrochemical kinetic analysis. The capacities of the final stabilization stage are provided by the reactions of reversible transformation between Na2S and S, which were considered the reaction mechanisms of Na-S batteries. This work can provide a basis for the synthesis and application of sulfur-rich compounds in fields of batteries, semiconductor devices, and catalysts.

15.
Mikrochim Acta ; 186(12): 784, 2019 11 15.
Artigo em Inglês | MEDLINE | ID: mdl-31732809

RESUMO

It is demonstrated that vanadium tetrasulfide (VS4) exhibits peroxidase (POx)-like activity which follows Michaelis-Menten kinetics when using H2O2 as a co-substrate. Electron spin resonance spectroscopy was use to analyze the catalytic mechanism. It suggests that the enzyme mimicking activity is caused by decomposing H2O2 into hydroxyl radicals. The method was used to quantify H2O2 by using 3,3',5,5'-tetramethylbenzidine as the substrate which results in the formation of a blue coloration (with an absorption peak at 652 nm). H2O2 can be detected in the 50 to 300 µM concentration range, and the detection limit is 5.0 µM. The assay for L-cysteine (L-cys) is based on the capability of oxTMB to oxidize L-cys to form L-cystine. The colorimetric L-cys assay has a linear response in the 5 to 100 µM concentration range and a 2.5 µM detection limit. Graphical abstractSchematic representation of the enzyme mimicking activity of vanadium tetrasulfide (VS4) submicrospheres originated from the decomposition of hydrogen peroxide (H2O2) to generate reactive hydroxyl radical (·OH) and the colorimetric detection of L-cysteine.


Assuntos
Cisteína/análise , Peróxido de Hidrogênio/análise , Microesferas , Compostos de Vanádio/química , Benzidinas/química , Catálise , Colorimetria/métodos , Corantes/química , Cisteína/química , Peróxido de Hidrogênio/química , Cinética , Limite de Detecção , Oxirredução , Peroxidase/química
16.
Mikrochim Acta ; 186(3): 141, 2019 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-30707311

RESUMO

An electrochemical sensor is described for the determination of nilutamide (NLM) in biological fluids. A flexible mat of nitrogen-doped carbon nanofibers (NCNFs) was prepared by electrospinning. This was followed by carbonization and the growth of one-dimensional vanadium tetrasulfide (VS4) nanorods in the circumference of the NCNFs by a solvothermal route. The material was used to modify a glassy carbon electrode (GCE). Cyclic voltammetry and amperometry revealed an excellent electrocatalytic activity of the VS4/NCNF mat towards NLM at a working potential of - 0.57 V (vs Ag/AgCl). The modified GCE has a wide linear range (0.001-760 µM), a low limit of detection (90 pM), good stability, and fast response. It was used to detect NLM in spiked serum and urine samples. Graphical abstract Schematic presentation of a glassy carbon electrode (GCE) composed of free-standing nitrogen-doped carbon nanofibers decorated with vanadium tetrasulfide (Patronite) nanorods (VS4/NCNF). It was fabricated by electrospinning followed by stabilization and carbonization. The GCE responds to nilutamide (NLM) with excellent selectivity and nanomolar sensitivity.


Assuntos
Carbono/química , Imidazolidinas/sangue , Nanofibras/química , Nitrogênio/química , Neoplasias da Próstata/diagnóstico , Compostos de Vanádio/química , Antineoplásicos/sangue , Técnicas Biossensoriais , Técnicas Eletroquímicas , Eletrodos , Humanos , Limite de Detecção , Masculino , Nanocompostos/química , Nanotubos/química , Tamanho da Partícula , Sulfetos/química , Propriedades de Superfície
17.
ACS Appl Mater Interfaces ; 10(17): 14727-14734, 2018 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-29624045

RESUMO

VS4 anode materials with controllable morphologies from hierarchical microflower, octopus-like structure, seagrass-like structure to urchin-like structure have been successfully synthesized by a facile solvothermal synthesis approach using different alcohols as solvents. Their structures and electrochemical properties with various morphologies are systematically investigated, and the structure-property relationship is established. Experimental results reveal that Li+ ion storage behavior in VS4 significantly depends on physical features such as the morphology, crystallite size, and specific surface area. According to this study, electrochemical performance degrades on the order of urchin-like VS4 > octopus-like VS4 > seagrass-like VS4 > flower-like VS4. Among them, urchin-like VS4 demonstrates the best electrochemical performance benefiting from its peculiar structure which possesses large surface area that accommodates the volume change to a certain extent, and single-crystal thorns that provide fast electron transportation. Kinetic parameters derived from EIS spectra and sweep-rate-dependent CV curves, such as charge-transfer resistances, Li+ ion apparent diffusion coefficients and stored charge ratio of capacitive and intercalation contributions, both support this claim well. In addition, the EIS measurement was conducted during the first discharge/charge process to study the solid electrolyte interface (SEI) formation on urchin-like VS4 and kinetics behavior of Li+ ion diffusion. A better fundamental understanding on Li+ storage behavior in VS4 is promoted, which is applicable to other vanadium-based materials as well. This study also provides invaluable guidance for morphology-controlled synthesis tailored for optimal electrochemical performance.

18.
ACS Appl Mater Interfaces ; 9(46): 40317-40323, 2017 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-29096435

RESUMO

A general synthetic approach has been demonstrated to fabricate three-dimensional (3D) structured metal sulfides@graphene, employing few-layered sulfide nanostructures with expanded interlayer spacing of the (002) plane (e.g., 0.98 nm for MoS2 nanoclusters and 0.65 nm for VS4 nanoribbons) and electrically conductive graphene as ideal building blocks. Here, small molecules (thioacetamide) acting as both the sulfur source and, more importantly, the structure-directing agent adjusting the interlayer spacing are wisely selected, further contributing to a sufficient space for ultrafast Li+ ion intercalation. The appealing features of a mechanically robust backbone, ultrathin thickness, abundant exposure of interlayer edges, and good electrical conductivity in such 3D architectures are favorable for providing easy access for the electrolyte to the structures and offering a shortened diffusion length of Li+ when utilized for energy storage. As a proof of concept, the electrochemical behavior of the resulting 3D structured metal sulfides@graphene as an anode material of lithium ion batteries (LIBs) is systematically investigated. As a consequence, high specific capacities, long lifespans, and superior rate capabilities have been realized in such well-designed architectures, e.g. maintaining a specific capacity as high as 965 mAh g-1 for 120 cycles for VS4@graphene and 1100 mAh g-1 for 150 cycles for MoS2@graphene.

19.
Proc Natl Acad Sci U S A ; 112(46): E6265-73, 2015 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-26578786

RESUMO

Noninvasive, radiological image-based detection and stratification of Gleason patterns can impact clinical outcomes, treatment selection, and the determination of disease status at diagnosis without subjecting patients to surgical biopsies. We present machine learning-based automatic classification of prostate cancer aggressiveness by combining apparent diffusion coefficient (ADC) and T2-weighted (T2-w) MRI-based texture features. Our approach achieved reasonably accurate classification of Gleason scores (GS) 6(3 + 3) vs. ≥7 and 7(3 + 4) vs. 7(4 + 3) despite the presence of highly unbalanced samples by using two different sample augmentation techniques followed by feature selection-based classification. Our method distinguished between GS 6(3 + 3) and ≥7 cancers with 93% accuracy for cancers occurring in both peripheral (PZ) and transition (TZ) zones and 92% for cancers occurring in the PZ alone. Our approach distinguished the GS 7(3 + 4) from GS 7(4 + 3) with 92% accuracy for cancers occurring in both the PZ and TZ and with 93% for cancers occurring in the PZ alone. In comparison, a classifier using only the ADC mean achieved a top accuracy of 58% for distinguishing GS 6(3 + 3) vs. GS ≥7 for cancers occurring in PZ and TZ and 63% for cancers occurring in PZ alone. The same classifier achieved an accuracy of 59% for distinguishing GS 7(3 + 4) from GS 7(4 + 3) occurring in the PZ and TZ and 60% for cancers occurring in PZ alone. Separate analysis of the cancers occurring in TZ alone was not performed owing to the limited number of samples. Our results suggest that texture features derived from ADC and T2-w MRI together with sample augmentation can help to obtain reasonably accurate classification of Gleason patterns.


Assuntos
Processamento de Imagem Assistida por Computador/métodos , Aprendizado de Máquina , Imageamento por Ressonância Magnética , Neoplasias da Próstata/diagnóstico por imagem , Humanos , Masculino , Valor Preditivo dos Testes , Radiografia
20.
ACS Appl Mater Interfaces ; 7(37): 20902-8, 2015 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-26328897

RESUMO

As an alternative system of rechargeable lithium ion batteries, sodium ion batteries revitalize researchers' interest due to the low cost, abundant sodium resources, and similar storage mechanism to lithium ion batteries. VS4 has emerged as a promising anode material for SIBs due to low cost and its unique linear chains structure that can offer potential sites for sodium storage. Herein, we present the growth of VS4 on reduced graphene oxide (rGO) as SIBs anode for the first time. The VS4/rGO anode exhibits promising performance in SIBs. It delivers a reversible capacity of 362 mAh g(-1) at 100 mA g(-1) and a good rate performance. We also investigate the sodium storage behavior of the VS4/rGO. Different than most transition metal sulfides, the VS4/rGO composite experiences a three-step separation mechanism during the sodiation process (VS4 to metallic V and Na2S, then the electrochemical mechanism is akin to Na-S). The VS4/rGO composite proves to be a promising material for rechargeable SIBs.

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