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1.
Artigo em Inglês | MEDLINE | ID: mdl-32100367

RESUMO

Despite the fact that many strategies have been developed to improve the efficiency of the oxygen evolution reaction (OER), the precise modulation of the surface electronic properties of catalysts to improve their catalytic activity is still challenging. Herein, we demonstrate that the surface active electron density of Co3 O4 can be effectively regulated by an argon-ion irradiation method. X-ray photoelectron and synchrotron x-ray absorption spectroscopy, UV photoelectron spectrometry, and DFT calculations show that the surface active electron density band center of Co3 O4 has been upshifted, leading to a significantly enhanced absorption capability of the oxo group. The optimized Co3 O4 -based catalysts exhibit an excellent overpotential of 260 mV at 10 mA cm-2 and Tafel slope of 54 mV dec-1 , superior to the capability of the benchmark RuO2 , representing one of the best Co-based OER catalysts. This approach could guide the future rational design and discovery of ideal electrocatalysts.

2.
ACS Appl Mater Interfaces ; 12(4): 5136-5146, 2020 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-31894690

RESUMO

The protein phosphorylation status of exosomes can regulate the activity and function of proteins related to cancer development, and it is highly possible to diagnose cancers through analyzing the protein phosphorylation status. However, monitoring the protein phosphorylation status with a simple and label-free method is still clinically challenging. Here, inspired by beehives, we developed an Au-coated TiO2 macroporous inverse opal (MIO) structure with an engineered "slow light effect" and thus with outstanding surface-enhanced Raman scattering (SERS) performance. The MIO structure can capture and analyze the exosomes from plasma of cancer patients without any labeling processes. It was found that the SERS intensity of exosomes at 1087 cm-1 arising from the P-O bond within the phosphoproteins can be used as a criterion for tumor liquid biopsies. The intensity of the 1087 cm-1 SERS peak from exosomes extracted from the plasma of cancer patients (prostate, lung, liver, and colon) is at least two times of that from healthy people. This indicates the simplicity and versatility of this method in cancer diagnostics. Our method has obvious advantages (noninvasive and time-saving) over currently clinically used tumor liquid biopsy techniques (such as western blot), which has great potentials to make vitro cancer diagnostics/monitoring as simple as diagnostics/monitoring of common diseases.

3.
Small ; 16(5): e1905609, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31899596

RESUMO

All-inorganic halide perovskites (IHPs) have attracted enormous attention due to their intrinsically high optical absorption coefficient and superior ambient stabilities. However, the photosensitivity of IHP-based photodetectors is still restricted by their poor conductivities. Here, a facile design of hybrid phototransistors based on the CsPbBr3 thin film and indium tin oxide (ITO) nanowires (NWs) integrated into a InGaZnO channel in order to achieve both high photoresponsivity and fast response is reported. The metallic ITO NWs are employed as electron pumps and expressways to efficiently extract photocarriers from CsPbBr3 and inject electrons into InGaZnO. The obtained device exhibits the outstanding responsivity of 4.9 × 106 A W-1 , which is about 100-fold better than the previous best results of CsPbBr3 -based photodetectors, together with the fast response (0.45/0.55 s), long-term stability (200 h in ambient), and excellent mechanical flexibility. By operating the phototransistor in the depletion regime, an ultrahigh specific detectivity up to 7.6 × 1013 Jones is achieved. More importantly, the optimized spin-coating manufacturing process is highly beneficial for achieving uniform InGaZnO-ITO/perovskite hybrid films for high-performance flexible detector arrays. All these results can not only indicate the potential of these hybrid phototransistors but also provide a valuable insight into the design of hybrid material systems for high-performance photodetection.

4.
Artigo em Inglês | MEDLINE | ID: mdl-31971777

RESUMO

Metallic multilayered nanofilms have been extensively studied owing to their unique physical properties and applications. However, studies on the thermal conductivity and electrical resistivity of metallic multilayered nanofilms, as their important physical properties, are seldom reported. In this work, Cu/W multilayered nanofilms with periodic thickness varying from 6 to 150 nm were deposited by magnetron sputtering. The resistivities of the Cu/W multilayered nanofilms increase with the decrease of periodic thickness, especially when the periodic thickness is smaller than 37 nm. The resistivities of the multilayered nanofilms fit well with the Fuchs-Sondheimer and Mayadas-Shatzkes (FS-MS) model, which considers both interface scattering and grain boundary scattering. The thermal conductivities of the Cu/W multilayered nanofilms were measured by the three-omega (3ω) method, which decrease with a decrease of periodic thickness initially and increase at the smallest periodic thickness of 6 nm. The Boltzmann transport equation (BTE)-based model was used, to explain the periodic thickness-dependent thermal conductivity of metallic multilayered nanofilms by considering the contributions from both phonon and electron heat transport processes, where the calculated thermal conductivities agree well with the measured ones. The electrical resistivity and thermal conductivity strongly depend on the microstructures of the multilayered nanofilms.

5.
Nanotechnology ; 31(14): 144002, 2020 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-31860888

RESUMO

Resistive switching devices have tremendous potential for memory, logic, and neuromorphic computing applications. Cation-based resistive switching devices intrinsically show nonvolatile memory characteristics under high compliance current (I CC), while show volatile threshold switching (TS) selector characteristics under low I CC. However, separate researches about cation-based memory or selector are hard to evade the typical current-retention dilemma, which results in the hardship to obtain low-current memory and high-current selector. Here, we propose a novel strategy to realize nonvolatile storage characteristics in a volatile TS device by modulating the rupture degree of conductive filament (CF). Enlarging the rupture degree of the CF with a certain RESET process, as confirmed by transmission electron microscope and energy dispersive spectrometry results, the threshold voltage of the Ag/HfO2/Pt TS devices can be enlarged from 0.9 to 2.8 V. Generation of the voltage difference enables the volatile TS devices the ability of self-selective nonvolatile storage. Increasing the RESET magnitude and shrinking the device size have been proved effective ways to increase the read window of the TS memory (TSM) devices. Evading the limit of the current-retention dilemma, ultra-low energy dissipation can be obtained by decreasing I CC to nA level. With self-selective, low-energy, and potential high-density integration characteristics, the proposed TSM device can act as a potential supplement of novel storage class memories.

6.
Angew Chem Int Ed Engl ; 58(46): 16660-16667, 2019 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-31489768

RESUMO

An N-doped TiO2 model reveals a conceptually different mechanism for activating the N dopant based on delocalized orbital hybridization through O vacancy incorporation. Synchrotron-based X-ray absorption spectroscopy, time-resolved fluorescence, and DFT studies revealed that O vacancy incorporation can effectively stimulate the delocalization of N impurity states through p-band orbital modulation, which leads to a significant enhancement in photocarrier lifetime. Consequently, this effect also results in a remarkable increase in the incident photon-to-electron conversion efficiency in the range of 400-550 nm compared to that of conventional N-incorporated TiO2 (15 % versus 1 % at 450 nm). This work reveals the fundamental necessity of orbital modulation in the band engineering of metal oxides for driving solar water splitting and beyond.

7.
Materials (Basel) ; 12(17)2019 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-31438471

RESUMO

Developing high-radiation-tolerant inert matrix fuel (IMF) with a long lifetime is important for advanced fission nuclear systems. In this work, we combined zirconia (ZrO2) with magnesia (MgO) to form ultrafine-grained ZrO2-MgO composite ceramics. On the one hand, the formation of phase interfaces can stabilize the structure of ZrO2 as well as inhibiting excessive coarsening of grains. On the other hand, the grain refinement of the composite ceramics can increase the defect sinks. Two kinds of composite ceramics with different grain sizes were prepared by spark plasma sintering (SPS), and their radiation damage behaviors were evaluated by helium (He) and xenon (Xe) ion irradiation. It was found that these dual-phase composite ceramics had better radiation tolerance than the pure yttria-stabilized ZrO2 (YSZ) and MgO. Regarding He+ ion irradiation with low displacement damage, the ZrO2-MgO composite ceramic with smaller grain size had a better ability to manage He bubbles than the composite ceramic with larger grain size. However, the ZrO2-MgO composite ceramic with a larger grain size could withstand higher displacement damage in the phase transformation under heavy ion irradiation. Therefore, the balance in managing He bubbles and phase stability should be considered in choosing suitable grain sizes.

8.
Nanoscale ; 11(15): 7041-7061, 2019 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-30931460

RESUMO

Flexible solid-state supercapacitors possess promising safety performance and intrinsic fast charging-discharging properties, enabling them to accomplish the requirements of lightweight and multifunctional wearable electronics that have recently become fairly popular. Because electrode materials are the core component of flexible solid-state supercapacitors, we exhaustively review the recent investigations involving electrode materials that have used carbons, metal oxides, and conductive polymers. The principles and methods of optimizing and fabricating electrodes for use in flexible supercapacitors are discussed through a comprehensive analysis of the literature. In addition, we focused on three types of flexible solid-state supercapacitors (fiber-, paper-, and porous foam-based structures) to satisfy the requirements of flexible electronic devices. Further, we summarize the practical applications of flexible solid-state supercapacitors, including energy conversion/collection devices and energy storage/detection devices. Finally, we provide the developmental direction for flexible solid-state supercapacitors in the future.

9.
Small ; 15(11): e1805516, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30706645

RESUMO

Virus detection and analysis are of critical importance in biological fields and medicine. Surface-enhanced Raman scattering (SERS) has shown great promise in small molecule and even single molecule detection, and can provide fingerprint signals of molecules. Despite the powerful detection capabilities of SERS, the size discrepancy between the SERS "hot spots" (generally, <10 nm) and viruses (usually, sub-100 nm) yields poor detection reliability of viruses. Inspired by the concept of molecular imprinting, a volume-enhanced Raman scattering (VERS) substrate composed of hollow nanocones at the bottom of microbowls (HNCMB) is developed. The hollow nanocones of the resulting VERS substrates serve a twofold purpose: 1) extending the region of Raman signal enhancement from the nanocone surface (e.g., surface "hot spots") to the hollow area within the cone (e.g., volume "hot spots")-a novel method of Raman signal enhancement, and 2) directing analyte such as viruses of a wide range of sizes to those VERS "hot spots" while simultaneously increasing the surface area contributing to SERS. Using HNCMB VERS substrates, greatly improved Raman signals of single viruses are demonstrated, an achievement with important implications in disease diagnostics and monitoring, biomedical fields, as well as in clinical treatment.

10.
Nanoscale Res Lett ; 14(1): 35, 2019 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-30684022

RESUMO

For an economical use of solar energy, photocatalysts that are sufficiently efficient, stable, and capable of harvesting light are required. Composite heterostructures composed of noble metals and semiconductors exhibited the excellent in catalytic application. Here, 1D Ag/Au/AgCl hollow heterostructures are synthesized by galvanic replacement reaction (GRR) from Ag nanowires (NWs). The catalytic properties of these as-obtained Ag/Au/AgCl hollow heterostructures with different ratios are investigated by reducing 4-nitrophenol (Nip) into 4-aminophenol (Amp) in the presence of NaBH4, and the influence of AgCl semiconductor to the catalytic performances of Ag/Au bimetals is also investigated. These hollow heterostructures show the higher catalytic properties than pure Ag NWs, and the AgCl not only act as supporting materials, but the excess AgCl is also the obstacle for contact of Ag/Au bimetals with reactive species. Moreover, the photocatalytic performances of these hollow heterostructures are carried out by degradation of acid orange 7 (AO7) under UV and visible light. These Ag/Au/AgCl hollow heterostructures present the higher photocatalytic activities than pure Ag NWs and commercial TiO2 (P25), and the Ag/Au bimetals enhance the photocatalytic activity of AgCl semiconductor via the localized surface plasmon resonance (LSPR) and plasmon resonance energy transfer (PRET) mechanisms. The as-synthesized 1D Ag/Au/AgCl hollow heterostructures with multifunction could apply in practical environmental remedy by catalytic manners.

11.
Front Chem ; 6: 580, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30525027

RESUMO

Exploring highly active, enduringly stable, and low-cost oxygen evolution reaction catalysts continues to be a dominant challenge to commercialize renewable electrochemical water-splitting technology. High-active and earth-abundant cobalt phosphides are recently considered as promising candidates. However, the poor inherent electron transfer efficiency and instability hinder its further development. In this work, a novel approach was demonstrated to effectively synthesize Co2P nanoparticles wrapped in amorphous porous carbon framework (Co2P/C). Benefiting from extremely high specific surface area of porous carbon, plenty of active sites were adequately exposed. Meanwhile, unique anchoring structure between Co2P nanoparticles and amorphous carbon outerwear insured high charge transfer efficiency and superior stability of Co2P/C. Due to these favorable properties, low overpotential of 281 mV at 10 mA cm-2 and Tafel slope of 69 mV dec-1 were achieved in resultant Co2P/C catalyst. More significantly, it only exhibited a negligible overpotential increase after 30 h stability test, and these performances entirely preceded commercial RuO2 benchmark. In summary, we proposed a simple and feasible strategy to prepare metal phosphides wrapped with amorphous porous carbon outerwear for efficient and durable electrochemical water oxidation.

12.
ACS Appl Mater Interfaces ; 10(30): 25737-25743, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29978695

RESUMO

Mercury ion (Hg2+) is one of the most toxic heavy metals that has severe adverse effects on the environment and human organs even at very low concentrations. Therefore, highly sensitive and selective detection of Hg2+ is desirable. Here, we introduce plasmonic micropinball constructed from Au nanooctahedron as a three-dimensional surface-enhanced Raman spectroscopy (SERS) platform, enabling ultrasensitive detection of trace Hg2+ ions. Typically, strong SERS signals could be obtained when the single-stranded DNA structure converts to the hairpin structure in the presence of Hg2+ ions, due to the formation of thymine (T)-Hg2+-T. As a result, the detection limit of Hg2+ ions is as low as 1 × 10-16 M, which is far below compared to that reported for conventional analytical strategies. Moreover, to achieve rapid multiple detection, we combine the micropinball sensors with microflow tube online detection. Our platform prevents cross-talk and tube contamination, allowing multiassay analysis, rapid identification, and quantification of different analytes and concentrations across separate phases.

13.
Nanotechnology ; 29(15): 155301, 2018 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-29384492

RESUMO

Here we reported the fabrication of tungsten oxide (WO3-x ) nanowires by Ar+ ion irradiation of WO3 thin films followed by annealing in vacuum. The nanowire length increases with increasing irradiation fluence and with decreasing ion energy. We propose that the stress-driven diffusion of the irradiation-induced W interstitial atoms is responsible for the formation of the nanowires. Comparing to the pristine film, the fabricated nanowire film shows a 106-fold enhancement in electrical conductivity, resulting from the high-density irradiation-induced vacancies on the oxygen sublattice. The nanostructure exhibits largely enhanced surface-enhanced Raman scattering effect due to the oxygen vacancy. Thus, ion irradiation provides a powerful approach for fabricating and tailoring the surface nanostructures of semiconductors.

14.
Nanotechnology ; 29(18): 184005, 2018 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-29451496

RESUMO

The metal-oxide semiconductor TiO2 shows enormous potential in the field of photoelectric detection; however, UV-light absorption only restricts its widespread application. It is considered that nitrogen doping can improve the visible light absorption of TiO2, but the effect of traditional chemical doping is far from being used for visible light detection. Herein, we dramatically broadened the absorption spectrum of the TiO2 nanowire (NW) by nitrogen ion implantation and apply the N-doped single TiO2 NW to visible light detection for the first time. Moreover, this novel strategy effectively modifies the surface states and thus regulates the height of Schottky barriers at the metal/semiconductor interface, which is crucial to realizing high responsivity and a fast response rate. Under the illumination of a laser with a wavelength of 457 nm, our fabricated photodetector exhibits favorable responsivity (8 A W-1) and a short response time (0.5 s). These results indicate that ion implantation is a promising method in exploring the visible light detection of TiO2.

15.
ACS Appl Mater Interfaces ; 9(46): 40726-40733, 2017 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-29086549

RESUMO

The ability to enhance the heat resistance of noble metals is vital to many industrial and academic applications. Because of its exceptional thermal properties, graphene was used to enhance the thermal stability of noble metals. Monolayer graphene-covered noble metal triangular nanoarrays (TNAs) showed excellent heat resistance, which could maintain their original triangular nanoarrays at high temperatures, whereas bare noble metal TNAs all agglomerate into spherical nanoparticles. On the basis of this mechanism, we obtained a universal recyclable surface-enhanced Raman scattering (SERS) substrate; after 16 cycles, the SERS substrate still worked well. The improvement of the heat resistance of noble metals by graphene has a great significance to the working reliability and service life of electronic devices and the single-use problem of traditional SERS substrates.

16.
ACS Appl Mater Interfaces ; 9(16): 14534-14544, 2017 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-28398034

RESUMO

Surface-enhanced Raman spectroscopy (SERS) is a versatile and powerful spectroscopic technique for substance analysis and detection. So far, the highest detection sensitivities have been realized on noble nanostructure substrates, which, however, are costly, unstable, and non-biocompatible. While semiconductor substrates could in principle be used, existing realizations have either resulted in substrates with low sensitivities or used methods that have poor technical control. Here we report a general and versatile method, based on ion irradiation and vacuum annealing, for fabricating large-scale reduced semiconducting oxide SERS substrates with high sensitivities. The SERS enhancement mainly stems from oxygen vacancy-associated electronic states created by the ion irradiation of sample; these states enhance the charge-transfer (CT) mechanism between the oxide substrate and the adsorbed molecules and thus significantly magnify SERS signals. The improved carrier mobility by vacuum annealing and the introduction of impurity energy levels and nanostructures enhances further the CT efficiency. A detection limit as low as 5 × 10-8 M was achieved; this is the highest sensitivity among the reported semiconductors, and it even compares to noble metals without the aid of "hot spots". The method is general-we demonstrate it on WO3, ZnO, and TiO2 substrates using Ar+ and N+ ion beam irradiation-and broadly applicable to produce noble-metal-free SERS substrates with high sensitivities.

17.
Nanoscale Res Lett ; 12(1): 221, 2017 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-28340531

RESUMO

Flower-like MoS2 nanoparticles (NPs) consist of ultra-thin MoS2 nanosheets are synthesized via a facile one-pot hydrothermal method. The MoS2/ZnO p-n heterostructure is formed by coating n-type ZnO on the surface of flower-like MoS2 NPs through the seed-mediate route and post-annealing treatment. The effects for the dye removal and photocatalytic performances after ZnO coating are systematically investigated. The results demonstrated that the coating of ZnO nanoparticles has a positive promotion to the photodegrading properties while negative effect on the adsorption capacity of the MoS2/ZnO heterostructures. The related mechanisms on the relationship of adsorption capacity and photocatalysis are discussed in detail.

18.
ACS Appl Mater Interfaces ; 9(12): 10798-10804, 2017 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-28266830

RESUMO

Despite intensive research on improvement in electrical performances of ZnO-based thin-film transistors (TFTs), the instability issues have limited their applications for complementary electronics. Herein, we have investigated the effect of nitrogen and hydrogen (N/H) codoping on the electrical performance and reliability of amorphous InGaZnO (α-IGZO) TFTs. The performance and bias stress stability of α-IGZO device were simultaneously improved by N/H plasma treatment with a high field-effect mobility of 45.3 cm2/(V s) and small shifts of threshold voltage (Vth). On the basis of X-ray photoelectron spectroscopy analysis, the improved electrical performances of α-IGZO TFT should be attributed to the appropriate amount of N/H codoping, which could not only control the Vth and carrier concentration efficiently, but also passivate the defects such as oxygen vacancy due to the formation of stable Zn-N and N-H bonds. Meanwhile, low-frequency noise analysis indicates that the average trap density near the α-IGZO/SiO2 interface is reduced by the nitrogen and hydrogen plasma treatment. This method could provide a step toward the development of α-IGZO TFTs for potential applications in next-generation high-definition optoelectronic displays.

19.
Sci Rep ; 7: 43901, 2017 03 02.
Artigo em Inglês | MEDLINE | ID: mdl-28252106

RESUMO

Nanostructured Si as the high efficiency photoelectrode material is hard to keep stable in aqueous for water splitting. Capping a passivation layer on the surface of Si is an effective way of protecting from oxidation. However, it is still not clear in the different mechanisms and effects between insulating oxide materials and oxide semiconductor materials as passivation layers. Here, we compare the passivation effects, the photoelectrochemical (PEC) properties, and the corresponding mechanisms between the HfO2/nanoporous-Si and the TiO2/nanoporous-Si by I-V curves, Motte-schottky (MS) curves, and electrochemical impedance spectroscopy (EIS). Although the saturated photocurrent densities of the TiO2/nanoporous Si are lower than that of the HfO2/nanoporous Si, the former is more stable than the later.

20.
Nanoscale ; 9(9): 3114-3120, 2017 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-28203665

RESUMO

Low-cost, stabilized and ultrasensitive three-dimensional (3D) hierarchical surface-enhanced Raman scattering substrates ("sunflower-like" nanoarrays decorated with Ag nanoparticles, denoted as SLNAs-Ag) have been obtained by fabricating binary colloidal crystals and then decorating with Ag nanoparticles. In order to provide a larger density of hot spots within the laser-illumination area, the silica sphere arrays were chosen as the island-type platform for the polystyrene (PS) nanosphere deposition, and the distances between the PS nanospheres were tuned by etching for different durations. Compared with conventional 2D planar systems, the as-fabricated 3D SLNAs-Ag exhibited extremely high SERS sensitivity ascribed to the larger SERS active regions. Quantitative detection of molecules with an extremely low incident laser power was achieved on the "sunflower-like" nanoarrays in which the PS nanospheres were etched for 5 minutes and decorated with Ag nanoparticles, and the corresponding analytical enhancement factor is calculated to be 2 × 1014 with the concentration of rhodamine 6G down to 10-15 M. Based on the achieved SERS substrates, we have further demonstrated the highly sensitive detection of molecules such as melamine for food safety inspection.

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