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1.
Inorg Chem ; 63(9): 4312-4327, 2024 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-38354197

RESUMEN

It is crucial to eliminate CO emissions using non-noble catalysts. Cu-based catalysts have been widely applied in CO oxidation, but their activity and stability at low temperatures are still challenging. This study reports the preparation and application of an efficient copper-doped ceria electrospun fiber catalyst prepared by a facile electrospinning method. The obtained 10Cu-Ce fiber catalyst achieved complete CO oxidation at a temperature as low as 90 °C. However, a reference 10Cu/Ce catalyst prepared by the impregnation method needed 110 °C to achieve complete CO oxidation under identical reaction conditions. Asymmetric oxygen vacancies (ASOV) at the interface between copper and cerium were constructed, to effectively absorb gas molecules involved in the reaction, leading to the enhanced oxidation of CO. The exceptional ability of the 10Cu-Ce catalyst to adsorb CO is attributed to its unique structure and surface interaction phase Cu+-Ov-Ce3+, as demonstrated by a series of characterizations and DFT calculations. This novel approach of using electrospinning offers a promising technique for developing low-temperature and non-noble metal-based catalysts.

2.
Small ; 19(15): e2206940, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36604989

RESUMEN

It is indispensable to develop and design high capacity, high rate performance, long cycling life, and low-cost electrodes materials for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). Herein, MoO2 /MoS2 /C, with dual heterogeneous interfaces, is designed to induce a built-in electric field, which has been proved by experiments and theoretical calculation can accelerate electrochemical reaction kinetics and generate interfacial interactions to strengthen structural stability. The carbon foam serves as a conductive frame to assist the movement of electrons/ions, as well as forms heterogeneous interfaces with MoO2 /MoS2 through CS and CO bonds, maintaining structural integrity and enhancing electronic transport. Thanks to these unique characteristics, the MoO2 /MoS2 /C renders a significantly enhanced electrochemical performance (324 mAh g-1 at 1 A g-1 after 1000 cycles for SIB and 500 mAh g-1 at 1 A g-1 after 500 cycles for LIBs). The current work presents a simple, useful and cost-effective route to design high-quality electrodes via interfacial engineering.

3.
Appl Opt ; 62(24): 6528-6533, 2023 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-37706847

RESUMEN

A large lateral photovoltaic effect (LPE) with a fast optical response time is necessary to develop high-performance position-sensitive detectors. In this paper, we report an LPE with a high self-powered position sensitivity and ultrafast optical relaxation time in S n S 2/n-S i junctions prepared using pulsed laser deposition. A large built-in electric field was generated at the S n S 2/S i interface, which resulted in a large LPE with a positional sensitivity of up to 116 mV/mm. Furthermore, the measurement circuit with multiple parallel resistors had a strong influence on the ultrafast optical response time of the LPE and the fastest optical relaxation time observed was ∼0.44µs. Our results suggest that the S n S 2/S i junction would be a promising candidate for a wide range of optoelectronic device applications.

4.
Molecules ; 28(1)2022 Dec 30.
Artículo en Inglés | MEDLINE | ID: mdl-36615510

RESUMEN

Water electrolysis offers a zero-carbon route to generate renewable energy conversion systems. Herein, a self-supported nickel phosphosulfide nanosheet (NS) electrocatalyst was fabricated at a low temperature on carbon cloth, which was then subjected to Ar etching to enhance its catalytic activity. Etching resulted in better hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance than other samples, with overpotentials of 103.1 mV (at 10 mA cm-2) and 278.9 mV (at 50 mA cm-2), respectively. The characterization results confirmed that Ar etching created a thin amorphous layer around the NiPS3 NSs, which increased the number of active sites and modulated their electronic structures. These 3D-structured NiPS3 NSs and their subsequent Ar etching process show promise for applications in overall water splitting in alkaline media.

5.
Nanotechnology ; 32(3): 035601, 2021 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-33089831

RESUMEN

The controllable growth of high-quality transition metal dichalcogenides (TMDs) is crucial for their device applications, which rely on the atomic and quantitative understanding of the growth mechanism of TMDs. In this work, we propose a comprehensive picture of the growth of WS2 nanosheets via Monte Carlo simulation, and an extension of diffusion-limited growth under transition state theory is developed to describe heteroepitaxy growth of WS2. Theoretical results are in good agreement with the results of chemical vapor deposition that growth temperature dominates growth processes leading to samples with various densities of vacancy defects. The vacancy defects modify the photoluminescence and ferromagnetic behavior. Our work provides a pathway toward realizing controllable physical properties in 2D materials.

6.
Angew Chem Int Ed Engl ; 60(1): 259-267, 2021 Jan 04.
Artículo en Inglés | MEDLINE | ID: mdl-32964599

RESUMEN

To ensure sustainable hydrogen production by water electrolysis, robust, earth-abundant, and high-efficient electrocatalysts are required. Constructing a hybrid system could lead to further improvement in electrocatalytic activity. Interface engineering in composite catalysts is thus critical to determine the performance, and the phase-junction interface should improve the catalytic activity. Here, we show that nickel diphosphide phase junction (c-NiP2 /m-NiP2 ) is an effective electrocatalyst for hydrogen production in alkaline media. The overpotential (at 10 mA cm-2 ) for NiP2 -650 (c/m) in alkaline media could be significantly reduced by 26 % and 96 % compared with c-NiP2 and m-NiP2 , respectively. The enhancement of catalytic activity should be attributed to the strong water dissociation ability and the rearrangement of electrons around the phase junction, which markedly improved the Volmer step and benefited the reduction process of adsorbed protons.

7.
Appl Opt ; 58(19): 5200-5205, 2019 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-31503614

RESUMEN

Optoelectronic position-sensitive detectors (PSDs) based on the lateral photovoltaic effect (LPE) have been a focus of research due to their ability to detect very small displacements. In this paper, we investigate the LPE properties of MoSe2/p-Si junctions prepared using pulsed laser deposition. The LPE shows a good linear dependence with the position of the laser spot. A large positional sensitivity and a fast optical relaxation time of 563 mV mm-1 and 2 µs, respectively, were observed in the MoSe2 (10 nm)/p-Si junction. The influence of the laser power and the wavelength on the LPE suggests that the observed response originates from the photoelectric effect. The large positional sensitivity and fast relaxation time of the LPE make the MoSe2/p-Si junction a promising candidate for PSDs.

8.
Opt Express ; 26(26): 34214-34223, 2018 Dec 24.
Artículo en Inglés | MEDLINE | ID: mdl-30650852

RESUMEN

A large lateral photovoltaic (LPV) effect with good linearity and fast response time is necessary for developing high-performance position-sensitive detectors (PSD). In this paper, we investigated the influence of the resistance of Sb2Se3 film and the Si on the LPV properties of the Sb2Se3/p-Si junctions. The LPV exhibits a linear dependence on the laser spot position, with a maximum position sensitivity as high as 448 mV/mm. The optical relaxation time of the LPV was about 4.98 µs, which was due to the formation of the inversion layer at the Sb2Se3/p-Si interface. Our results revealed that the high resistivity of Sb2Se3 film facilitate the LPV and confirmed the resistivity of Si substrate play a key role in the LPV properties. The giant position sensitivity and fast relaxation times of the LPV suggest that the Sb2Se3/p-Si junction is a promising candidate for a wide range of optoelectronic device applications.

9.
Opt Express ; 25(19): 23283-23292, 2017 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-29041629

RESUMEN

Oceanic turbulence is described by the oceanic refractive-index spectrum (ORIS), which considers several important hydrodynamic parameters. Based on ORIS, many optical oceanic quantities can be calculated using numerical integration. However, it is difficult to calculate the analytical solutions. In this paper, an approximate oceanic temperature spectrum is obtained by multiplying the non-Kolmogorov spectrum with a correction factor. By analogy with the obtained temperature spectrum, an approximate salinity spectrum and an approximate coupling spectrum are obtained. A linear summation of these three approximate spectra forms the approximate form of ORIS. The approximate form of ORIS we obtained helps calculate the analytical solutions of the relevant oceanic optical quantities.

10.
Nanotechnology ; 28(27): 275703, 2017 Jul 07.
Artículo en Inglés | MEDLINE | ID: mdl-28597845

RESUMEN

To safely and reliably use aluminum nitride (AlN) helices in the fabrication of novel micro/nanodevices, it is very important to know their mechanical properties. Herein, we investigate the mechanical properties of individual AlN helices using an in situ tensile-bending test. Tensile tests reveal that an AlN helix has an average ε of ∼4.7 ± 0.8% elastic deformation before a typical brittle fracture occurs. The bending test shows a two-step mechanical feature-linear-elastic followed by an elastic-plastic process-with an average ε bent of ∼54.5 ± 0.6%. Our results provide direct cognition about the mechanical properties of AlN helices and their benefit to the design of AlN-based flexible micro/nanodevices.

11.
J Am Chem Soc ; 138(25): 7965-72, 2016 06 29.
Artículo en Inglés | MEDLINE | ID: mdl-27269185

RESUMEN

Molybdenum disulfide (MoS2) is a promising nonprecious catalyst for the hydrogen evolution reaction (HER) that has been extensively studied due to its excellent performance, but the lack of understanding of the factors that impact its catalytic activity hinders further design and enhancement of MoS2-based electrocatalysts. Here, by using novel porous (holey) metallic 1T phase MoS2 nanosheets synthesized by a liquid-ammonia-assisted lithiation route, we systematically investigated the contributions of crystal structure (phase), edges, and sulfur vacancies (S-vacancies) to the catalytic activity toward HER from five representative MoS2 nanosheet samples, including 2H and 1T phase, porous 2H and 1T phase, and sulfur-compensated porous 2H phase. Superior HER catalytic activity was achieved in the porous 1T phase MoS2 nanosheets that have even more edges and S-vacancies than conventional 1T phase MoS2. A comparative study revealed that the phase serves as the key role in determining the HER performance, as 1T phase MoS2 always outperforms the corresponding 2H phase MoS2 samples, and that both edges and S-vacancies also contribute significantly to the catalytic activity in porous MoS2 samples. Then, using combined defect characterization techniques of electron spin resonance spectroscopy and positron annihilation lifetime spectroscopy to quantify the S-vacancies, the contributions of each factor were individually elucidated. This study presents new insights and opens up new avenues for designing electrocatalysts based on MoS2 or other layered materials with enhanced HER performance.

12.
Opt Express ; 24(21): 23755-23764, 2016 Oct 17.
Artículo en Inglés | MEDLINE | ID: mdl-27828212

RESUMEN

In this paper, we report a sensitive lateral photovoltaic effect (LPE) in Fe3O4/3C-SiC Schottky junctions with a fast relaxation time at near-ultraviolet wavelengths. The rectifying behavior suggests that the large build-in electric field was formed in the Schottky junctions. This device has excellent position sensitivity as high as 67.8 mV mm-1 illuminated by a 405 nm laser. The optical relaxation time of the LPE is about 30 µs. The fast relaxation and high positional sensitivity of the LPE make the Fe3O4/3C-SiC junction a promising candidate for a wide range of ultraviolet/near-ultraviolet optoelectronic applications.

13.
Nano Lett ; 15(10): 6575-81, 2015 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-26372072

RESUMEN

The coupling effect between nitrogen-vacancies (VN) and aluminum-interstitial sites (Ali) is investigated theoretically and experimentally in AlN helices. First-principles calculations predict a photoluminescence emission peak at approximately 600 nm in AlN doped with complex-defect (VNAli). A typical long afterglow (persistent luminescence) was observed in unintentionally doped AlN helices by introducing the complex-defect of (VNAli). An analysis of the luminescent characteristics indicated that the mechanism behind this afterglow is the complex-defect level and complex-defect density. These findings may further enrich the thoughts of defects in the wide band gap semiconductor of AlN.


Asunto(s)
Aluminio/química , Difracción de Rayos X
14.
Phys Chem Chem Phys ; 16(38): 20828-33, 2014 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-25167075

RESUMEN

In this paper, we report on the hydrogen photochromism in Nb2O5 powders with different structures. Four different powder phases were prepared by calcining Nb2O5·nH2O powders at various temperatures, and their morphology, structure, and electronic band structure were characterized by scanning electron microscopy, structural analyses, thermogravimetric analysis, differential scanning calorimetry, and optical spectroscopy. Nb2O5 powders with different structures and very different properties were formed after different high-temperature treatments of the polymorphous oxide. A pronounced photochromic effect was observed in the M and H phases of Nb2O5, whereas the other phases exhibited poor photochromic responses. Because photochromism arises due to the detachment of hydrogen atoms under the action of light from hydrogen donor molecules previously adsorbed on the oxide surface, the electronic band structure and the morphology have strong influences on the photochromic properties of Nb2O5 powders. For these reasons, a pronounced photochromic effect was achieved in the H phase.

15.
ACS Appl Mater Interfaces ; 16(8): 10138-10147, 2024 Feb 28.
Artículo en Inglés | MEDLINE | ID: mdl-38364211

RESUMEN

Enhancing the reaction selectivity for multicarbon products (C2+) is an important goal for the electrochemical CO(2) reduction (ECO(2)R) process. Cuprous compounds have demonstrated promising C2+ selectivity in the ECO(2)R process, but further investigation is necessary to thoroughly elucidate their catalytic behavior toward C2+ oxygenate production. In this study, copper nitride-based materials with varying reduction rates were employed as precatalysts. Consequently, a relationship between the selectivity toward C2+ oxygenates and the Cu oxidation state during the ECOR process is established. Results of theoretical and experimental analyses reveal that the Cu0/Cu+ interface plays a key role in enhancing *CO adsorption while lowering the formation energy of *CH2CO, thereby promoting acetate production. This work highlights the significance of the Cu0/Cu+ interface in the regulation of C2+ oxygenate production and paves the way for the development of highly selective catalysts in the future.

16.
ACS Appl Mater Interfaces ; 16(21): 27813-27820, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38603540

RESUMEN

Solar-blind photodetectors based on wide bandgap semiconductors have recently attracted a lot of interest. Nickel-containing spinel phase oxides, such as NiAl2O4, are stable p-type semiconductors. This paper describes a multifunctional solar-blind photodetector based on a NiAl2O4/4H-SiC heterojunction that utilizes photovoltaic effects. The position sensitivity reaches a value of 1589.7 mV/mm under 405 nm laser illumination, while the relaxation times of vertical photovoltaic (VPV) effect and lateral photovoltaic (LPV) effect under 266 nm laser illumination are only 0.32 and 0.42 µs, respectively. This junction was used to create a space optical communication system with sunlight having little effect on its optoelectronic properties. The ultrafast photovoltaic relaxation time makes NiAl2O4/4H-SiC a promising candidate for self-powered high-performance solar-blind detectors.

17.
Environ Sci Ecotechnol ; 20: 100405, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38544949

RESUMEN

The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies. Sulfate radical-based advanced oxidation has emerged as an attractive solution, offering high selectivity, enduring efficacy, and anti-interference ability. Among many technologies, sulfite activation, leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates, stands out. Yet, the activation process often relies on transition metals, suffering from low atom utilization. Here we introduce a series of single-atom catalysts (SACs) employing transition metals on g-C3N4 substrates, effectively activating sulfite for acetaminophen degradation. We highlight the superior performance of Fe/CN, which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN. Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency, with oxysulfur radical-mediated reactions predominating. Notably, under visible light, the catalytic activity is enhanced, attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic. The proximity of Fe/CN's d-band center to the Fermi level, alongside its high spin polarization, is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap, thereby accelerating photo-assisted sulfite activation. This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.

18.
ACS Appl Mater Interfaces ; 15(1): 1505-1512, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36548398

RESUMEN

CsPbBr3, an inorganic halide perovskite, has attracted great interest in recent years due to its excellent photoelectric properties. In this paper, we report a high-performance position-sensitive detector and laser communication sensor based on a CsPbBr3/4H-SiC heterojunction that effectively exploits the lateral photovoltaic (LPV) effect. The X-ray diffraction, X-ray photoelectron spectra, and photoluminescence data indicate that a high-quality CsPbBr3 film has been successfully obtained using pulsed laser deposition. The thickness of the CsPbBr3 film is shown to play a key role in the open-circuit voltage and linear LPV. A large position sensitivity (up to 827 mV/mm) of the LPV with a fast relaxation time is observed. Moreover, the shortest relaxation time of only 0.34 µs for 532 nm laser irradiation among counterparts is achieved in the detector under consideration. Furthermore, the position sensitivity and relaxation time of the LPV in the CsPbBr3/4H-SiC heterojunction show a weak dependence on the laser wavelength from 266 to 532 nm. The robust characteristics of fast relaxation time and high position sensitivity of the LPV make the CsPbBr3 junction a promising candidate for both laser communication sensors and self-powered high-performance position-sensitive detectors.

19.
Materials (Basel) ; 15(11)2022 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-35683174

RESUMEN

Designing a high-strength node is significant for space structures. Topological optimization can optimally allocate the material distribution of components to meet performance requirements. Although the material distribution after topology optimization is optimum, the structure becomes complicated to manufacture. By using additive manufacturing technology, this problem can be well solved. At present, both topology optimization technology and additive manufacturing technology are quite mature, but their application in the design of spatial nodes is very recent and less researched. This paper involves the study and improvement of the node optimization design-manufacturing integrated method. This study used the BESO optimization algorithm as the research algorithm. Through a reasonable improvement of the material interpolation method, the algorithm's dependence on the experience of selecting the material penalty index P was reduced. On this basis, the secondary development was carried out, and a multisoftware integration was carried out for optimization and manufacturing. The spatial node was taken as the research object, and the calculation results of the commercial finite element software were compared. The comparison showed that the algorithm used in this paper was better. Not only was it not trapped in a local optimum, but the maximum stress was also lower. In addition, this paper proposed a practical finite element geometric model extraction method and smoothing of the optimized nodes, completing the experiment of the additive manufacturing forming of the nodes. It provides ideas for processing jagged edges brought by the BESO algorithm. This paper verified the feasibility of the multisoftware integration method of optimized manufacturing.

20.
Small Methods ; 6(6): e2200084, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35460208

RESUMEN

Here, a strategy to regulate the electron density distribution by integrating NiFe layered double hydroxides (NiFe-LDH) nanosheets with Co3 O4 nanowires to construct the NiFe-LDH/Co3 O4 p-n heterojunction supported on nickel foam (NiFe-LDH/Co3 O4 /NF) for electrocatalytic oxygen evolution reaction (OER) is proposed. The p-n heterojunction can induce the charge redistribution in the heterogeneous interface to reach Fermi level alignment, thus modifying the adsorption free energy of *OOH and improving the intrinsic activity of the catalyst. As a result, NiFe-LDH/Co3 O4 /NF exhibits outstanding OER performance with a low overpotential of 274 mV at a current density of 50 mA cm-2 and long-time stability over 90 h. Moreover, NF can serve as a magnetic core that induces the exchange bias effect between the magnetic substrate and the active species under the action of the magnetic field, resulting in decreased magnetoresistance and weakened scattering of spin electrons, which further lowers the OER overpotential by 25 mV @ 50 mA cm-2 under a 10 000 G magnetic field. This work provides a new perspective on the design of p-n heterojunction catalysts and a deeper understanding of the magnetic field-enhanced electrocatalytic reactions.

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