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1.
Small ; : e2401530, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38751307

RESUMEN

The unavoidable and unpredictable surface reconstruction of metallic copper (Cu) during the electrocatalytic carbon dioxide (CO2) reduction process is a double-edged sword affecting the production of high-value-added hydrocarbon products. It is crucial to control the surface facet reconstruction and regulate the targeted facets/facet interfaces, and further understand the mechanism between activity/selectivity and the reconstructed structure of Cu for CO2 reduction. Based on the current catalyst design methods, a facile strategy combining chemical reduction and electro-reduction is proposed to achieve specified Cu(111) facets and the Cu(110)/(111) interfaces in reconstructed Cu derived from cuprous oxide (Cu2O). The surface facet reconstruction significantly boosted the electrocatalytic conversion of CO2 into multi-carbon (C2+) products comparing to the unmodified catalyst. Theoretical and experimental analyses show that the Cu(110)/(111)s interface between Cu(110) and a small amount of Cu(111) can tailor the reaction routes and lower the reaction energy barrier of C-C coupling to ethylene (C2H4). The work will guide the surface facets reconstruction strategy for Cu-based CO2 electrocatalysts, providing a promising paradigm to understand the structural variation in catalysts.

2.
Adv Mater ; : e2403792, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38742953

RESUMEN

Seawater electrolysis is a potentially cost-effective approach to green hydrogen production, but it currently faces substantial challenges for its high energy consumption and the interference of chlorine evolution reaction (ClER). Replacing the energy-demanding oxygen evolution reaction with methanol oxidation reaction (MOR) represents a promising alternative, as MOR occurs at a significantly low anodic potential, which cannot only reduce the voltage needed for electrolysis but also completely circumvents ClER. To this end, developing high-performance MOR catalysts is a key. Herein, a novel quaternary Pt1.8Pd0.2CuGa/C intermetallic nanoparticle (i-NP) catalyst is reported, which shows a high mass activity (11.13 A mgPGM -1), a large specific activity (18.13 mA cmPGM -2), and outstanding stability toward alkaline MOR. Advanced characterization and density functional theory calculations reveal that the introduction of atomically distributed Pd in Pt2CuGa intermetallic markedly promotes the oxidation of key reaction intermediates by enriching electron concentration around Pt sites, resulting in weak adsorption of carbon-containing intermediates and favorable adsorption of synergistic OH- groups near Pd sites. MOR-assisted seawater electrolysis is demonstrated, which continuously operates under 1.23 V for 240 h in simulated seawater and 120 h in natural seawater without notable degradation.

3.
ACS Appl Mater Interfaces ; 15(38): 45465-45474, 2023 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-37709730

RESUMEN

Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is a highly promising solid-state lithium metal battery electrolyte due to its exceptional ionic conductivity and electrochemical stability. However, when exposed to air, a passivation layer can be spontaneously formed on the garnet-type electrolyte, deteriorating its wettability with metallic lithium (Li) and impeding the lithium ion transfer at the Li-garnet electrolyte interface. The passivation layer is considered a critical issue for garnet-type solid electrolytes. Despite intensive research, the formation mechanism of the passivation film remains poorly understood. The key to elucidating the formation mechanism is to obtain a pristine garnet electrolyte surface and study how the pristine garnet electrolyte interacts with air. In this study, different passivation layer removal pretreatments were performed to expose pristine garnet electrolytes, and their impacts on the samples were systematically studied. The results reveal the overlooked negative impacts of vacuum annealing and acid treatment on LLZTO, which are indicated by the severe loss of Li and O and the formation of additional Li-depleted metal oxides. It was confirmed that argon annealing is the only viable approach to remove the passivation layer without introducing concomitant contaminations to LLZTO. Based on this method, we directly evidenced the formation of LiOH on LLZTO under rarefied air using quasi-in situ X-ray photoelectron spectroscopy. It was confirmed that the loss of Li and O ions, rather than Li+/H+ exchange, drives the formation of LiOH in the passivation layer. These results not only provide a better understanding of the surface and interface chemistry of LLZTO but also reveal a reliable surface treatment for the LLZTO sample.

4.
J Colloid Interface Sci ; 650(Pt B): 1715-1724, 2023 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-37499627

RESUMEN

Although Pt is a widely adopted commercial catalyst for the hydrogen evolution reaction (HER), its practical application is greatly limited by its prohibitive cost and high energy barrier for H2O dissociation in alkaline media. Herein, an ultrafine Pt-based catalyst decorated with oxygenophilic Ni-sites is rationally designed and successfully synthesized with Pt5(GS)10 (HGS = l-reduced glutathione) nanocluster precursor. The optimized Ni-decorated Pt catalyst (Ni-Pt-C-500) with ultrafine nanoparticles (about 1.6 nm) exhibits a low overpotential (14.0 mV) at 10 mA cm-2 and a mild Tafel slope of 20.8 mV dec-1 in the HER, which is superior to its undecorated counterpart (Pt-C-500), the commercial 20 wt% Pt/C catalyst and most of the previously reported Pt-based electrocatalysts. Experimental observations and theoretical calculations indicate that H2O could be spontaneously adsorbed to Ni-sites of the Ni-Pt-C-500 catalyst. Mechanistic studies reveal that Ni-sites promote HER by accelerating the kinetic of H2O cleavage and optimizing the electronic structure of Pt. This work paves a new avenue for designing other ultrafine hybrid electrocatalysts based on metal nanoclusters to enhance catalytic reaction kinetics.

5.
J Mol Model ; 29(3): 68, 2023 Feb 16.
Artículo en Inglés | MEDLINE | ID: mdl-36792837

RESUMEN

CONTEXT: Using chemical penetration enhancers to improve the penetration effect is one kind of important strategies in transdermal drug delivery system. Azone is a widely used transdermal absorption enhancer for transdermal drug delivery. To shed light on the permeation-promoting mechanism of azone, we selected ternary systems formed by azacyclopentane-2-one and N-methylolacetamide (1: 2) and explored the synergetic effect of hydrogen-bonding interactions among them and their thermodynamic properties. The findings indicate that the synergetic effects can enhance the ability of azone to change the original conformation of ceramides and even break the original hydrogen bonds, which is more beneficial for azone to destroy the 3D network structure of ceramides. When azone interacts with ceramide, the order of action tends to interact with one molecule of ceramide first and then with another molecule of ceramide. METHODS: The synergetic effects of hydrogen-bonding interactions in ternary systems were computed at the B3LYP/6-311 + + G** and MP2(full)/6-311 + + G** levels. Thermodynamic parameters for two ternary-complex routes were worked out at the B3LYP/aug-cc-pVDZ level. The shift of the electron density occurring simultaneously with trimer formation was analyzed at the MP2(full)/6-311 + + G** level. The above calculations were carried out using the Gaussian 03 program packages. Atoms in molecules (AIM) method and the AIMPAC program showed the topological charge density at the MP2(full)/6-311 + + G** level. The synergetic effects of hydrogen-bonding interactions and thermodynamic property in the 1: 2 (azacyclopentane-2-one: N-methylolacetamide) ternary systems were investigated using the B3LYP and MP2(full) methods.

6.
Small Methods ; 6(9): e2200636, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35879051

RESUMEN

Hydrogen production from water electrolysis is important for the sustainable development of hydrogen energy. Nevertheless, the naturally torpid property of anodic oxygen evolution reaction (OER) kinetics and poor stability of its catalysts significantly restrict the development of electrochemical water splitting. Here, a Ru0.6 Cr0.4 O2 electrocatalyst is synthesized, which reveals excellent OER activity with the overpotential of only 195 mV at 10 mA cm-2 and excellent stability with the potential increase of merely 5.3 mV after 20 h continuous OER test in acidic media. Theoretical calculations reveal that the solubilizing of Cr into RuO2 could adjust the electron distribution, making the d-band center of Ru far away from the Fermi level. This behavior reduces the binding energy with Ru and O and accelerates the rate-determining step of OER (i.e., the formation of *OOH), thereby increasing OER activity. In addition, the incorporation of Cr increases the energy of oxygen defect formation and reduces the participation of lattice oxygen, thus improving the stability of the catalyst. This research furnishes a feasible policy for the development of highly active and stable catalysts in acidic media by regulating the electronic structure of RuO2 .

7.
Drug Dev Res ; 83(4): 1034-1046, 2022 06.
Artículo en Inglés | MEDLINE | ID: mdl-35277867

RESUMEN

Preeclampsia (PE) is one of the most serious diseases during pregnancy. Circular RNAs (circRNAs) are strongly related to the occurrence of preeclampsia. Herein, we aimed to explore the potential role and mechanism of circRNA oligophrenin 1 (circ-OPHN1; hsa_circ_0007445) in PE. Quantitative real-time polymerase chain reaction (qPCR) and western blot were utilized to detect gene expression levels. The biological behaviors of trophoblast cells were determined by 3-(4,5-dimethyl-2-thiazolyl)-2,5-diphenyl-2-H-tetrazolium bromide (MTT), flow cytometry, transwell, and wound healing methods. The binding relationship between microRNA-558 (miR-558) and circ-OPHN1 or thrombospondin 2 (THBS2) was validated via dual-luciferase reporter assay. Circ-OPHN1 and THBS2 levels were enhanced, while miR-558 level was declined in PE placental tissues. Circ-OPHN1 or THBS2 overexpression hindered the proliferation, migration, and invasion of trophoblast cells. In addition, circ-OPHN1 sequestered miR-558 to regulate THBS2 expression, thereby repressing the growth and mobility of trophoblast cells. Circ-OPHN1 inhibited trophoblast cell proliferation, migration, and invasion through mediating miR-558/THBS2 axis, providing a novel pathway for PE pathogenesis.


Asunto(s)
MicroARNs , Preeclampsia , ARN Circular , Trombospondinas , Trofoblastos , Movimiento Celular , Proliferación Celular , Proteínas del Citoesqueleto/metabolismo , Femenino , Proteínas Activadoras de GTPasa/metabolismo , Humanos , MicroARNs/genética , Proteínas Nucleares/metabolismo , Placenta/metabolismo , Placenta/patología , Preeclampsia/genética , Embarazo , ARN Circular/genética , Trombospondinas/genética , Trombospondinas/metabolismo , Trofoblastos/metabolismo , Trofoblastos/patología
8.
Small Methods ; 5(6): e2100246, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-34927904

RESUMEN

The development of cost-effective electrocatalysts with high activity and sufficient stability for hydrogen evolution reaction (HER) is crucial for the widespread application of water electrolysis for sustainable H2 production. Transition metal oxides are desirable alternatives to replace benchmark Pt-based HER electrocatalysts because of their cost effectiveness, facile synthesis, versatile compositions, and easy electronic structure tuning. However, most available transition metal oxides show poor performance for HER catalysis. Here, it is reported that the anatase TiO2 can be efficiently developed into a superior HER electrocatalyst with comparable activity to Pt-based electrocatalysts in alkaline solution through simultaneous morphology control, proper lattice doping, and surface active sites engineering. Specifically, the obtained cobalt-doped TiO2 nanorod arrays (Co-TiO2 @Ti(H2 )) show a low overpotential of only 78 mV at 10 mA cm-2 , a small Tafel plot of 67.8 mV dec-1 , and excellent stability even at an ultralarge current density of ≈480 mA cm-2 in 1.0 m KOH solution. Theoretical calculations demonstrate that the introduction of Co with rich oxygen vacancies can efficiently lower the energy barrier for water adsorption/dissociation and H intermediate desorption. This work uncovers the potential of the low-cost transition metal oxides as alternative HER electrocatalysts in alkaline water electrolysis.

9.
Chem Soc Rev ; 50(2): 1138-1187, 2021 Jan 21.
Artículo en Inglés | MEDLINE | ID: mdl-33245736

RESUMEN

High temperature proton exchange membrane fuel cells (HT-PEMFCs) are one type of promising energy device with the advantages of fast reaction kinetics (high energy efficiency), high tolerance to fuel/air impurities, simple plate design, and better heat and water management. They have been expected to be the next generation of PEMFCs specifically for application in hydrogen-fueled automobile vehicles and combined heat and power (CHP) systems. However, their high-cost and low durability interposed by the insufficient performance of key materials such as electrocatalysts and membranes at high temperature operation are still the challenges hindering the technology's practical applications. To develop high performance HT-PEMFCs, worldwide researchers have been focusing on exploring new materials and the related technologies by developing novel synthesis methods and innovative assembly techniques, understanding degradation mechanisms, and creating mitigation strategies with special emphasis on catalysts for oxygen reduction reaction, proton exchange membranes and bipolar plates. In this paper, the state-of-the-art development of HT-PEMFC key materials, components and device assembly along with degradation mechanisms, mitigation strategies, and HT-PEMFC based CHP systems is comprehensively reviewed. In order to facilitate further research and development of HT-PEMFCs toward practical applications, the existing challenges are also discussed and several future research directions are proposed in this paper.

10.
Small ; 16(44): e2004188, 2020 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-33043586

RESUMEN

In order to further overcome the shortage of electrodes with additive/binder and modulate the structure of NiCo2 O4 for supercapacitors, ultrathin NiCo2 O4 nanosheet arrays have been in situ grown on Ni foam by optimizing hydrothermal reactions based on crystal growth dynamics. The structure of ultrathin NiCo2 O4 nanosheet arrays can expose more active sites, provide abundant diffusion channels and buffer the stress caused by phase transition during charge-discharge process of supercapacitors. The optimized hydrothermal reactions can provide more ordered crystal orientations by keeping nanosheets on Ni foam completely coming from in situ growth, which will decrease the inner resistance of ultrathin NiCo2 O4 nanosheets and improve the efficiency and kinetics of electrons transfer. By the virtue of such remarkable features, the electrochemical results confirm the rationality of structural modulation and crystal orientations optimization with a drastically enhanced specific capacitance of 2017.8 F g-1 , admirable rate performance of 93.2% and outstanding stability retention of 90.9% after cycling 5000 times. More impressively, the assembled flexible solid-state asymmetric supercapacitor (ASC) shows superior energy density, power density, and high stability. The modification strategy in this paper may throw light on the rational design of new generation advanced electrode materials for high-performance flexible supercapacitors.

11.
Chem Commun (Camb) ; 56(81): 12109-12121, 2020 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-32959823

RESUMEN

The electroproduction of H2O2 through 2e oxygen reduction reaction (ORR) as an alternative strategy for the conventional anthraquinone process is highly energy-efficient and environment-friendly. Different kinds of electrocatalysts with high selectivity, activity, and stability have been recently reported, and are an essential part of the whole electroproduction process of H2O2. In this review, we expound the ORR mechanism and introduce some methods to screen out potential electrocatalysts through theoretical calculations and experimental verifications. In addition, recent advances in reactor design for large-scale on-site production of H2O2 and integrated systems for electricity-H2O2 co-generation are mentioned. With ideal electrocatalysts and rational reactor design, different concentrations of H2O2 can be obtained depending on the practical applications. Utilizing the solar or chemical energy, it can promote energy efficiency and sustainability of the process. Finally, we make a brief conclusion about recent developments in electrocatalysts, device design, as well as integrated systems, and give an outlook for future research challenges, which are meaningful for advancing the electrochemical on-site production of H2O2via 2e ORR to the marketplace.

12.
Chem Commun (Camb) ; 56(72): 10529-10532, 2020 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-32780071

RESUMEN

A simple method is provided to achieve in situ surface reconstruction synthesis of a heterostructural NiO/Ni film on carbon cloth (NiO/Ni@CC) for the hydrogen evolution reaction (HER). This ultrafast reconstruction process brings a hydrophilic surface and abundant heterostructures with rich oxygen vacancies exhibiting a low HER overpotential and remarkable stability.

13.
Adv Sci (Weinh) ; 7(14): 2000407, 2020 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-32714753

RESUMEN

The rational design of electrode structure with catalysts adequately utilized is of vital importance for future fuel cells. Herein, a novel 3D oriented wholly integrated electrode comprising core-shell Fe3O4@N-doped-C (Fe3O4@NC) nanoparticles embedded into N-doped ordered interconnected hierarchical porous carbon (denoted as Fe3O4@NC/NHPC) is developed for the oxygen reduction reaction (ORR). The as-prepared catalyst possesses novel structure and efficient active sites. In rotating disk electrode measurements, the Fe3O4@NC/NHPC exhibits almost identical ORR electrocatalytic activity, superior durability, and much better methanol tolerance compared with the commercial Pt/C in acidic media. To the authors' knowledge, this is among the best non-precious-metal ORR catalysts reported so far. Importantly, the Fe3O4@NC/NHPC is successfully in situ assembled onto carbon paper by the electrophoresis method to obtain a well-designed 3D-ordered electrode. With improved mass transfer and maximized active sites for ORR, the 3D-oriented wholly integrated electrode shows superior performance to the one fabricated by the traditional method.

14.
Adv Sci (Weinh) ; 7(5): 1902830, 2020 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-32154075

RESUMEN

Rational design of unique pre-catalysts for highly active catalysts toward catalyzing the oxygen evolution reaction (OER) is a great challenge. Herein, a Co-derived pre-catalyst that allows gradual exposure of CoOOH that acts as the active center for OER catalysis is obtained by both phosphate ion surface functionalization and Mo inner doping. The obtained catalyst reveals an excellent OER activity with a low overpotential of 265 mV at a current density of 10 mA cm-2 and good durability in alkaline electrolyte, which is comparable to the majority of Co-based OER catalysts. Specifically, the surface functionalization produces lots of Co-PO4 species with oxygen vacancies which can trigger the surface self-reconstruction of pre-catalyst for a favorable OER reaction. Density functional theory calculations reveal that the Mo doping optimizes adsorption-free energy of *OOH formation and thus accelerates intrinsic electrocatalytic activity. Expanding on these explorations, a series of transition metal oxide pre-catalysts are obtained using this general design strategy. The work offers a fundamental understanding toward the correlation among surface-structure-activity for the pre-catalyst design.

15.
Small ; 15(42): e1903297, 2019 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-31448556

RESUMEN

Developing highly efficient electrocatalysts with earth abundant elements for oxygen evolution reaction (OER) is a promising way to store light or electrical energy in the form of chemical energy. Here, a new type of electrocatalyst with core-shell carbon/NiCo2 O4 double microtubes architecture is successfully synthesized through a hydrothermal method combined with the calcination process with wet tissues as the template and carbon resource. The outer NiCo2 O4 nanosheet arrays contain abundant defects, which come from reduction of the carbon in wet tissues. This indicates that carbon is a very excellent defect inducer. The inner carbon microtubes can act as the robust structure skeleton and these core-shell double microtubes provide abundant diffusion channels for oxygen and electrolyte, both of which contribute to improving the stability by avoiding damage to the electrode from produced O2 bubbles and the collapse of the outer NiCo2 O4 microtubes. Electrochemical results show that the electrode, core-shell carbon/NiCo2 O4 double microtubes loaded on carbon cloth, exhibits prominent electrocatalytic activity with an overpotential of only 168 mV at 10 mA cm-2 and a Tafel slope as low as 57.6 mV dec-1 in 1.0 mol L-1 KOH. This new type of electrocatalyst possesses great potential in water electrolyzers and rechargeable metal-air batteries.

16.
Biochem Biophys Res Commun ; 511(4): 921-925, 2019 04 16.
Artículo en Inglés | MEDLINE | ID: mdl-30853176

RESUMEN

BACKGROUND: Non-small cell lung cancer (NSCLC) is a highly aggressive malignancy with increasing incidence across the world. The role and mechanism of circular RNAs (circRNAs) in the pathogenesis of NSCLC have not been understood exactly. In this work, we aims to explore a novel NSCLC-associated circRNA, circ_0003645. METHODS: The expression profile of circ_0003645 was evaluated in NSCLC tissue specimens and cells. Additionally, the correlation between circ_0003645 and clinical features/patients' prognosis were investigated. Functionally, CCK-8, clone formation, flow cyometric and transwell assays were performed in two cell lines. Furthermore, dual-luciferase reporter and rescue experiments were carried out to elucidate the mechanism of circ_0003645. RESULTS: The data demonstrated an upregulation of circ_0003645 in patients' tissue specimens and cells. Overexpression of circ_0003645 in tissues was related to advanced TNM stages, positive lymph node invasion and unfavorable prognosis for the patients with NSCLC. In addition, gain and loss of function assays uncovered that circ_0003645 functioned as an oncogene in NSCLC cells. Moreover, circ_0003645 acted as a ceRNA to sponge miR-1179, which resulted in the elevation of TMEM14A expression and facilitated cell progression. CONCLUSIONS: This study indicates that circ_0003645 might possess crucial potential as a prognosis predictor and therapeutic target for NSCLC patients.


Asunto(s)
Proteínas Reguladoras de la Apoptosis/genética , Carcinoma de Pulmón de Células no Pequeñas/genética , Regulación Neoplásica de la Expresión Génica , Neoplasias Pulmonares/genética , Proteínas de la Membrana/genética , MicroARNs/genética , ARN Circular/genética , Carcinoma de Pulmón de Células no Pequeñas/diagnóstico , Carcinoma de Pulmón de Células no Pequeñas/patología , Línea Celular Tumoral , Progresión de la Enfermedad , Femenino , Humanos , Neoplasias Pulmonares/diagnóstico , Neoplasias Pulmonares/patología , Masculino , Persona de Mediana Edad , Pronóstico , Regulación hacia Arriba
17.
J Mol Model ; 24(6): 139, 2018 May 31.
Artículo en Inglés | MEDLINE | ID: mdl-29855720

RESUMEN

The structures of the N-(hydroxymethyl)acetamide (model molecule of ceramide) dimers have been fully optimized at B3LYP/6-311++G** level. The intermolecular hydrogen bonding interaction energies have been calculated using the B3LYP/6-311++G**, B3LYP/6-311++G(2df,2p), MP2(full)/6-311++G** and MP2(full)/6-311++G(2df,2p) methods, respectively. The results show that the O-H···O, N-H···O, O-H···N, and C-H···O hydrogen bonding interactions could exist in N-(hydroxymethyl)acetamide dimers, and the O-H···O, N-H···O, and O-H···N hydrogen bonding interactions could be stronger than C-H···O. The three-dimensional network structure formed by ceramide molecules through intermolecular hydrogen bonding interactions may be the main reason why the stratum corneum of skin could prevent foreign substances from entering our body, as is in accordance with the experimental results. The stability of hydrogen-bonding interactions follow the order of (a) > (b) ≈ (c) > (d) > (e) ≈ (f) > (g) > (h). The analyses of the energy decomposition, frequency, atoms in molecules (AIM), natural bond orbital (NBO), and electron density shift are used to further reveal the nature of the complex formation. In the range of 263.0-328.0 K, the complex is formed via an exothermic reaction, and the solvent with lower temperature and dielectric constant is favorable to this process. Graphical abstract The structures and the O-H···O=C, N-H···O=C and C-H···O=C H-bonding interactions in the N-(hydroxymethyl)acetamide (model molecule of ceramide) dimers were investigated using the B3LYP and MP2(full) methods.

18.
Small ; 13(41)2017 11.
Artículo en Inglés | MEDLINE | ID: mdl-28895281

RESUMEN

Recently, researchers have made significant advancement in employing transition metal compound hybrids as anode material for lithium-ion batteries and developing simple preparation of these hybrids. To this end, this study reports a facile and scalable method for fabricating a vanadium oxide-nitride composite encapsulated in amorphous carbon matrix by simply mixing ammonium metavanadate and melamine as anode materials for lithium-ion batteries. By tuning the annealing temperature of the mixture, different hybrids of vanadium oxide-nitride compounds are synthesized. The electrode material prepared at 700 °C, i.e., VM-700, exhibits excellent cyclic stability retaining 92% of its reversible capacity after 200 cycles at a current density of 0.5 A g-1 and attractive rate performance (220 mAh g-1 ) under the current density of up to 2 A g-1 . The outstanding electrochemical properties can be attributed to the synergistic effect from heterojunction form by the vanadium compound hybrids, the improved ability of the excellent conductive carbon for electron transfer, and restraining the expansion and aggregation of vanadium oxide-nitride in cycling. These interesting findings will provide a reference for the preparation of transition metal oxide and nitride composites as well.

19.
ACS Appl Mater Interfaces ; 8(43): 29356-29364, 2016 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-27718543

RESUMEN

Identifying non-precious-metal catalysts with desirable overall performance for oxygen reduction reaction (ORR) in either acidic or basic media is still a bottleneck. Here, a hybrid material is reported, in which tungsten carbide (WC) and ferberite (FeWO4) are attached to the Fe and N dual-doped ordered mesoporous carbon (WC-FeWO4@FeN-OMC) as a superior performance catalyst for the ORR in either acidic or basic media. In comparison with the frequently used Pt/C ORR catalyst (20 wt. %), our hybrid materials exhibit comparable electrocatalytic activity mainly via a 4e ORR process, better stability, and total tolerance to methanol in either acidic or basic media. These advantages, especially the outstanding stability in acidic media, render the WC-FeWO4@FeN-OMC as a promising potential non-precious-metal ORR catalyst in practical fuel cell applications.

20.
ACS Appl Mater Interfaces ; 6(15): 13174-82, 2014 Aug 13.
Artículo en Inglés | MEDLINE | ID: mdl-25025228

RESUMEN

Novel hierarchically porous carbon materials with very high surface areas, large pore volumes and high electron conductivities were prepared from silk cocoon by carbonization with KOH activation. The prepared novel porous carbon-encapsulated sulfur composites were fabricated by a simple melting process and used as cathodes for lithium sulfur batteries. Because of the large surface area and hierarchically porous structure of the carbon material, soluble polysulfide intermediates can be trapped within the cathode and the volume expansion can be alleviated effectively. Moreover, the electron transport properties of the carbon materials can provide an electron conductive network and promote the utilization rate of sulfur in cathode. The prepared carbon-sulfur composite exhibited a high specific capacity and excellent cycle stability. The results show a high initial discharge capacity of 1443 mAh g(-1) and retain 804 mAh g(-1) after 80 discharge/charge cycles at a rate of 0.5 C. A Coulombic efficiency retained up to 92% after 80 cycles. The prepared hierarchically porous carbon materials were proven to be an effective host matrix for sulfur encapsulation to improve the sulfur utilization rate and restrain the dissolution of polysulfides into lithium-sulfur battery electrolytes.


Asunto(s)
Biopolímeros/química , Carbono/química , Suministros de Energía Eléctrica , Litio/química , Azufre/química , Adsorción , Animales , Espectroscopía Dieléctrica , Conductividad Eléctrica , Técnicas Electroquímicas , Electroquímica , Electrodos , Nitrógeno/química , Tamaño de la Partícula , Porosidad , Seda/química , Temperatura , Termogravimetría , Difracción de Rayos X
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