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1864条结果
  • 机译 由非晶碳薄膜制造用于电子束成形的相位掩模
    摘要:Background: Electron-beam shaping opens up the possibility for novel imaging techniques in scanning (transmission) electron microscopy (S(T)EM). Phase-modulating thin-film devices (phase masks) made of amorphous silicon nitride are commonly used to generate a wide range of different beam shapes. An additional conductive layer on such a device is required to avoid charging under electron-beam irradiation, which induces unwanted scattering events. Results: Phase masks of conductive amorphous carbon (aC) were successfully fabricated with optical lithography and focused ion beam milling. Analysis by TEM shows the successful generation of Bessel and vortex beams. No charging or degradation of the aC phase masks was observed. Conclusion: Amorphous carbon can be used as an alternative to silicon nitride for phase masks at the expense of a more complex fabrication process. The quality of arbitrary beam shapes could benefit from the application of phase masks made of amorphous C.
  • 机译 基于粘土纳米结构的用于电化学装置的多组分生物纳米复合材料
    摘要:Based on the unique ability of defibrillated sepiolite (SEP) to form stable and homogeneous colloidal dispersions of diverse types of nanoparticles in aqueous media under ultrasonication, multicomponent conductive nanoarchitectured materials integrating halloysite nanotubes (HNTs), graphene nanoplatelets (GNPs) and chitosan (CHI) have been developed. The resulting nanohybrid suspensions could be easily formed into films or foams, where each individual component plays a critical role in the biocomposite: HNTs act as nanocontainers for bioactive species, GNPs provide electrical conductivity (enhanced by doping with MWCNTs) and, the CHI polymer matrix introduces mechanical and membrane properties that are of key significance for the development of electrochemical devices. The resulting characteristics allow for a possible application of these active elements as integrated multicomponent materials for advanced electrochemical devices such as biosensors and enzymatic biofuel cells. This strategy can be regarded as an “a la carte” menu, where the selection of the nanocomponents exhibiting different properties will determine a functional set of predetermined utility with SEP maintaining stable colloidal dispersions of different nanoparticles and polymers in water.
  • 机译 基于表面改性的聚合物氮化碳纳米管的仿生纳米流体二极管
    摘要:A controllable ion transport including ion selectivity and ion rectification across nanochannels or porous membranes is of great importance because of potential applications ranging from biosensing to energy conversion. Here, a nanofluidic ion diode was realized by modifying carbon nitride nanotubes with different molecules yielding an asymmetric surface charge that allows for ion rectification. With the advantages of low-cost, thermal and mechanical robustness, and simple fabrication process, carbon nitride nanotubes with ion rectification have the potential to be used in salinity-gradient energy conversion and ion sensor systems.
  • 机译 基于Janus-micromotor的开关荧光传感器,用于主动TNT检测
    摘要:An active TNT (2,4,6-trinitrotoluene) catalytic sensor based on Janus upconverting nanoparticle (UCNP)-functionalized micromotor capsules, displaying “on–off” luminescence with a low limit of detection has been developed. The Janus capsule motors were fabricated by layer-by-layer assembly of UCNP-functionalized polyelectrolyte microcapsules, followed by sputtering of a platinum layer onto one half of the capsule. By catalytic decomposition of hydrogen peroxide to oxygen bubbles, the Janus UCNP capsule motors are rapidly propelled with a speed of up to 110 μm s−1. Moreover, the Janus motors display efficient on–off luminescent detection of TNT. Owing to the unique motion of the Janus motor with bubble generation, the likelihood of collision with TNT molecules and the reaction rate between them are increased, resulting in a limit of detection as low as 2.4 ng mL−1 TNT within 1 minute. Such bubble-propelled Janus UCNP capsule motors have great potential for contaminated water analysis.
  • 机译 通过动态原子力显微镜对机械性能进行纳米尺度空间映射
    摘要:Dynamic atomic force microscopy (AFM) was employed to spatially map the elastic modulus of highly oriented pyrolytic graphite (HOPG), specifically by using force modulation microscopy (FMM) and contact resonance (CR) AFM. In both of these techniques, a variation in the amplitude signal was observed when scanning over an uncovered step edge of HOPG. In comparison, no variation in the amplitude signal was observed when scanning over a covered step on the same surface. These observations qualitatively indicate that there is a variation in the elastic modulus over uncovered steps and no variation over covered ones. The quantitative results of the elastic modulus required the use of FMM, while the CR mode better highlighted areas of reduced elastic modulus (although it was difficult to convert the data into a quantifiable modulus). In the FMM measurements, single atomic steps of graphene with uncovered step edges showed a decrease in the elastic modulus of approximately 0.5%, which is compared with no change in the elastic modulus for covered steps. The analysis of the experimental data taken under varying normal loads and with several different tips showed that the elastic modulus determination was unaffected by these parameters.
  • 机译 磁晶各向异性对硬磁和软磁铁氧体纳米粒子性能的影响
    摘要:Recent advances in the field of magnetic materials emphasize that the development of new and useful magnetic nanoparticles (NPs) requires an accurate and fundamental understanding of their collective magnetic behavior. Studies show that the magnetic properties are strongly affected by the magnetic anisotropy of NPs and by interparticle interactions that are the result of the collective magnetic behavior of NPs. Here we study these effects in more detail. For this purpose, we prepared CoxFe3− xO4 NPs, with x = 0–1 in steps of 0.2, from soft magnetic (Fe3O4) to hard magnetic (CoFe2O4) ferrite, with a significant variation of the magnetic anisotropy. The phase purity and the formation of crystalline NPs with a spinel structure were confirmed through Rietveld refinement. The effect of Co doping on structure, morphology and magnetic properties of CoxFe3− xO4 samples was investigated. In particular, we examined the interparticle interactions in the samples by δm graphs and Henkel plots that have not been reported before in literature. Finally, we studied the hyperthermia properties and observed that the heat efficiency of soft Fe3O4 is about 4 times larger than that of hard CoFe2O4 ferrite, which was attributed to the high coercive field of samples compared with the external field amplitude.
  • 机译 基于Au纳米颗粒/ CuBi2O4微棒的0D / 1D复合材料的构建,具有高效的可见光驱动的光催化活性
    摘要:Photocatalysis is considered to be a promising technique for the degradation of organic pollutants. Herein, a 0D/1D composite photocatalyst consisting of Au nanoparticles (NPs) and CuBi2O4 microrods (Au/CBO) was designed and prepared by a simple thermal reduction–precipitation approach. It shows excellent photocatalytic performance in the degradation of tetracycline (TC). The maximum photocatalytic degradation rate constant for Au/CBO composites with 2.5 wt % Au NPs was 4.76 times as high as that of bare CBO microrods. Additionally, the 0D/1D Au/CBO composite also exhibited ideal stability. The significant improvement of the photocatalytic performance could be attributed to the improved light harvesting and increased specific surface area, enhancing photoresponse and providing more active sites. Our work shows a possible design of efficient photocatalysts for environmental remediation.
  • 机译 含金纳米颗粒的有序介孔二氧化硅膜纳米复合材料,用于催化还原4-硝基苯酚
    摘要:We report that transparent mesostructured silica/gold nanocomposite materials with an interpore distance of 4.1 nm, as-synthesized from a templated sol–gel synthesis method using discotic trinuclear gold(I) pyrazolate complex, were successfully utilized for the fabrication of thin film mesoporous silica nanocomposites containing gold nanoparticles. The material exhibited a highly ordered hexagonal structure when subjected to a thermal hydrogen reduction treatment at 210 °C. In contrast, when the material was subjected to calcination as a heat treatment from 190 to 450 °C, the thin film nanocomposites showed an intense d 100 X-ray diffraction peak. Moreover, gold nanoparticles inside the thin film nanocomposites were confirmed by the presence of the d 111 diffraction peak at 2θ = 38.2°, a surface plasmon resonance peak between 500–580 nm, and the spherical shape observed in the transmission electron microscope images, as well as the visual change in color from pink to purple. Interestingly, by simply dipping the material into a reaction solution of 4-nitrophenol at room temperature, the highly ordered structure of the as-fabricated silica/gold nanoparticle thin film composite after thermal hydrogen reduction at 210 °C resulted in an improved catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol compared to the material calcined at 250 °C. Such catalytic activity is due to the presence of gold nanoparticles of smaller size in the silicate channels of the highly ordered mesoporous film nanocomposites.
  • 机译 单个SnO2纳米线和SnO2溶胶-凝胶纳米复合材料的气敏特性
    摘要:This work is an investigation of the properties of semiconductor materials based on metal oxides, their catalytic properties, and their application as gas sensors, which were shown to exhibit high sensitivity, stability, and selectivity to target gases. The aim of this work is the comparison of gas sensing properties of tin dioxide in the form of individual nanowires and nanopowders obtained by sol–gel synthesis. This comparison is necessary because the traditional synthesis procedures of small particle, metal oxide materials seem to be approaching their limit. Because of this, there is increasing interest in the fabrication of functional materials based on nanowires, i.e., quasi-one-dimensional objects. In this work, nanocrystalline tin dioxide samples with different morphology were synthesized. The gas-transport method was used for the fabrication of well-faceted wire-like crystals with diameters ranging between 15–100 nm. The sol–gel method allowed us to obtain fragile gels from powders with grain sizes of about 5 nm. By means of X-ray photoelectron spectroscopy (XPS) it was proven that the nanowires contain considerably smaller amounts of hydroxy groups compared to the nanopowders. This leads to a decrease in the parasitic sensitivity of the sensing materials to humidity. In addition, we demonstrated that the nanowires are characterized by a nearly single-crystalline structure, ensuring higher stability of the sensor response due to the unlikelihood of sample recrystallization. The results from the ammonia detection experiments showed that the ratio of the sensor response to the surface area exhibits similar values for both the individual nanowire and nanopowders-based sensor materials.
  • 机译 富勒烯萃取残留物氧化产生的翘曲石墨层及其氧还原催化活性
    摘要:Carbon-based oxygen reduction reaction (ORR) catalysts are regarded as a promising candidate to replace the currently used Pt catalyst in polymer electrolyte fuel cells (PEFCs); however, the active sites remain under discussion. We predicted that warped graphitic layers (WGLs) are responsible for the ORR catalytic activity in some carbon catalysts (i.e., carbon alloy catalysts (CACs)). To prove our assumption, we needed to use WGLs consisting of carbon materials, but without any extrinsic catalytic elements, such as nitrogen, iron, or cobalt, which effectively enhance ORR activity. The present study employed a fullerene extraction residue as a starting material to construct WGLs. The oxidation of the material at 600 °C exposed the WGLs by removing the surrounding amorphous moieties. Transmission electron microscopy (TEM) observations revealed the formation of WGLs by oxidation treatment at 600 °C in an O2/N2 stream. Extending the oxidation time increased the purity of the WGL phase, but also simultaneously increased the concentration of oxygen-containing surface functional groups as monitored by temperature programmed desorption (TPD). The specific ORR activity increased with oxidation up to 1 h and then decreased with the intensive oxidation treatment. Correlations between the specific ORR activity and other parameters confirmed that the development of the WGL and the increase in the O/C ratio are the competing factors determining specific ORR activity. These results explain the maximum specific ORR activity after 1 h of oxidation time. WGLs were found to lower the heat of adsorption for O2 and to increase the occurrence of heterogeneous electron transfer.
  • 机译 开尔文探针力显微镜在环境大气中的金属/半导体界面的纳米级表面电势势垒
    摘要:This study deals with the preparation and characterization of metallic nanoinclusions on the surface of semiconducting Bi2Se3 that could be used for an enhancement of the efficiency of thermoelectric materials. We used Au forming a 1D alloy through diffusion (point nanoinclusion) and Mo forming thermodynamically stable layered MoSe2 nanosheets through the reaction with the Bi2Se3. The Schottky barrier formed by the 1D and 2D nanoinclusions was characterized by means of atomic force microscopy (AFM). We used Kelvin probe force microscopy (KPFM) in ambient atmosphere at the nanoscale and compared the results to those of ultraviolet photoelectron spectroscopy (UPS) in UHV at the macroscale. The existence of the Schottky barrier was demonstrated at +120 meV for the Mo layer and −80 meV for the Au layer reflecting the formation of MoSe2 and Au/Bi2Se3 alloy, respectively. The results of both methods (KPFM and UPS) were in good agreement. We revealed that long-time exposure (tens of seconds) to the electrical field leads to deep oxidation and the formation of perturbations greater than 1 µm in height, which hinder the I–V measurements.
  • 机译 具有增强的可见光光催化活性的BiOCl / TiO2 /硅藻土复合材料降解罗丹明B
    摘要:A BiOCl/TiO2/diatomite (BTD) composite was synthesized via a modified sol–gel method and precipitation/calcination method for application as a photocatalyst and shows promise for degradation of organic pollutants in wastewater upon visible-light irradiation. In the composite, diatomite was used as a carrier to support a layer of titanium dioxide (TiO2) nanoparticles and bismuth oxychloride (BiOCl) nanosheets. The results show that TiO2 nanoparticles and BiOCl nanosheets uniformly cover the surface of diatomite and bring TiO2 and BiOCl into close proximity. Rhodamine B was used as the target degradation product and visible light (λ > 400 nm) was used as the light source for the evaluation of the photocatalytic properties of the prepared BTD composite. The results show that the catalytic performance of the BTD composite under visible-light irradiation is much higher than that of TiO2 or BiOCl alone. When the molar ratio of BiOCl to TiO2 is 1:1 and the calcination temperature is 400 °C, the composite was found to exhibit the best catalytic effect. Through the study of the photocatalytic mechanism, it is shown that the strong visible-light photocatalytic activity of the BTD composite results mainly from the quick migration of photoelectrons from the conduction band of TiO2/diatomite to the surface of BiOCl, which promotes the separation effect and reduces the recombination rate of the photoelectron–hole pair. Due to the excellent catalytic performance, the BTD composite shows great potential for wide application in the field of sewage treatment driven by solar energy.
  • 机译 使用Mn3O4 / WO3复合材料作为传感层的选择性气体检测
    摘要:Pure WO3 sensors and Mn3O4/WO3 composite sensors with different Mn concentrations (1 atom %, 3 atom % and 5 atom %) were successfully prepared through a facile hydrothermal method. As gas sensing materials, their sensing performance at different temperatures was systematically investigated for gas detection. The devices displayed different sensing responses toward different gases at specific temperatures. The gas sensing performance of Mn3O4/WO3 composites (especially at 3 atom % Mn) were far improved compared to sensors based on pure WO3, where the improvement is related to the heterojunction formed between the two metal oxides. The sensor based on the Mn3O4/WO3 composite with 3 atom % Mn showed a high selective response to hydrogen sulfide (H2S), ammonia (NH3) and carbon monoxide (CO) at working temperatures of 90 °C, 150 °C and 210 °C, respectively. The demonstrated superior selectivity opens the door for potential applications in gas recognition and detection.
  • 机译 直接观察电子辐照引起的Bi2WO6纳米片中氧空位的形成和结构变化
    摘要:The prominent role of oxygen vacancies in the photocatalytic performance of bismuth tungsten oxides is well recognized, while the underlying formation mechanisms remain poorly understood. Here, we use the transmission electron microscopy to investigate the formation of oxygen vacancies and the structural evolution of Bi2WO6 under in situ electron irradiation. Our experimental results reveal that under 200 keV electron irradiation, the breaking of relatively weak Bi–O bonds leads to the formation of oxygen vacancies in Bi2WO6. With prolonged electron irradiation, the reduced Bi cations tend to form Bi clusters on the nanoflake surfaces, and the oxygen atoms are released from the nanoflakes, while the W–O networks reconstruct to form WO3. A possible mechanism that accounts for the observed processes of Bi cluster formation and oxygen release under energetic electron irradiation is also discussed.
  • 机译 从溶液中生长氢化锂薄膜:向溶液原子层沉积锂化薄膜
    摘要:Lithiated thin films are necessary for the fabrication of novel solid-state batteries, including the electrodes and solid electrolytes. Physical vapour deposition and chemical vapour deposition can be used to deposit lithiated films. However, the issue of conformality on non-planar substrates with large surface area makes them impractical for nanobatteries the capacity of which scales with surface area. Atomic layer deposition (ALD) avoids these issues and is able to deposit conformal films on 3D substrates. However, ALD is limited in the range of chemical reactions, due to the required volatility of the precursors. Moreover, relatively high temperatures are necessary (above 100 °C), which can be detrimental to electrode layers and substrates, for example to silicon into which the lithium can easily diffuse. In addition, several highly reactive precursors, such as Grignard reagents or n-butyllithium (BuLi) are only usable in solution. In theory, it is possible to use BuLi and water in solution to produce thin films of LiH. This theoretical reaction is self-saturating and, therefore, follows the principles of solution atomic layer deposition (sALD). Therefore, in this work the sALD technique and principles have been employed to experimentally prove the possibility of LiH deposition. The formation of homogeneous air-sensitive thin films, characterized by using ellipsometry, grazing incidence X-ray diffraction (GIXRD), in situ quartz crystal microbalance, and scanning electron microscopy, was observed. Lithium hydride diffraction peaks have been observed in as-deposited films by GIXRD. X-ray photoelectron spectroscopy and Auger spectroscopy analysis show the chemical identity of the decomposing air-sensitive films. Despite the air sensitivity of BuLi and LiH, making many standard measurements difficult, this work establishes the use of sALD to deposit LiH, a material inaccessible to conventional ALD, from precursors and at temperatures not suitable for conventional ALD.
  • 机译 纳米粒子集合中的能量分布及其后果
    • 作者:Dieter Vollath
    • 刊名:Beilstein Journal of Nanotechnology
    • 2019年第期
    摘要:In general, considerations about isothermal ensembles of nanoparticles assume that each one of the particles is at the same temperature. However, there are experimental indications that such an isothermal ensemble does not exist. Therefore, it is advised to analyze phenomena connected to the temperature distribution within such an ensemble. The detailed analysis presented in this work led to the assumption of a normal distribution of the energy within an ensemble of nanoparticles where basic properties of such an “isothermal” ensemble can be predicted. The width of the energy distribution decreases with increasing particle size. This particle size dependence of the energy per particle controls phase fluctuations in the vicinity of the transformation temperature. Additionally, applying the temperature profile of a phase transformation, it is possible to calculate the particle size distribution of the ensemble with a precision within the scattering range of the experimental data. This is the most important application of this analysis and coincidently a proof of the basic premise. The basic quantity determining the width of the energy distribution is the heat capacity of the particles. For these calculations, bulk data for the heat capacity were successfully applied. This leads to the conclusion that the data for heat capacity of nanoparticles are very close to the bulk values.
  • 机译 碳纳米管掺杂液晶中的磁偏析效应
    摘要:We study the orientational transitions in a suspension of carbon nanotubes in a nematic liquid crystal induced by an external magnetic field. The case of a finite orientational anchoring of liquid crystal molecules at the surface of doped carbon nanotubes is considered. It is shown that in a magnetic field the initial homogeneous planar texture of the liquid crystal–carbon nanotubes mixture is disturbed in a threshold manner (Fréedericksz transition). The orientational and concentration distributions of the suspension are studied for different values of the magnetic field strength and segregation intensity of the impurity subsystem. The optical phase lag between ordinary and extraordinary rays of light transmitted through a layer of a liquid crystal composite is calculated. The possibility of changing the nature of the Fréedericksz transition from second order to first order is shown. This tricritical behavior is related to the redistribution of the carbon nanotubes (segregation effect) inside the layer.
  • 机译 用于电催化应用的分层结构3D碳纳米管电极
    摘要:Hierarchically structured 3-dimensional electrodes based on branched carbon nanotubes (CNTs) are prepared on a glassy carbon (GC) substrate in a sequence of electrodeposition and chemical vapor deposition (CVD) steps as follows: Primary CNTs are grown over electrodeposited iron by CVD followed by a second Fe deposition and finally the CVD growth of secondary CNTs. The prepared 3-dimensional CNT structures (CNT/CNT/GC) exhibit enhanced double-layer capacitance and thus larger surface area compared to CNT/GC. Pt electrodeposition onto both types of electrodes yields a uniform and homogeneous Pt nanoparticle distribution. Each preparation step is followed by scanning electron microscopy, while the CNTs were additionally characterized by Raman spectroscopy. In this way it is demonstrated that by varying the parameters during the electrodeposition and CVD steps, a tuning of the structural parameters of the hierarchical electrodes is possible. The suitability of the hierarchical electrodes for electrocatalytic applications is demonstrated using the methanol electro-oxidation as a test reaction. The Pt mass specific activity towards methanol oxidation of Pt-CNT/CNT/GC is approximately 2.5 times higher than that of Pt-CNT/GC, and the hierarchical electrode exhibits a more negative onset potential. Both structures demonstrate an exceptionally high poisoning tolerance.
  • 机译 基于MoS2的柔性独立式复合纸,用于能量转换和存储
    摘要:The construction of flexible electrochemical devices for energy storage and generation is of utmost importance in modern society. In this article, we report on the synthesis of flexible MoS2-based composite paper by high-energy shear force milling and simple vacuum filtration. This composite material combines high flexibility, mechanical strength and good chemical stability. Chronopotentiometric charge–discharge measurements were used to determine the capacitance of our paper material. The highest capacitance achieved was 33 mF·cm−2 at a current density of 1 mA·cm−2, demonstrating potential application in supercapacitors. We further used the material as a cathode for the hydrogen evolution reaction (HER) with an onset potential of approximately −0.2 V vs RHE. The onset potential was even lower (approximately −0.1 V vs RHE) after treatment with n-butyllithium, suggesting the introduction of new active sites. Finally, a potential use in lithium ion batteries (LIB) was examined. Our material can be used directly without any binder, additive carbon or copper current collector and delivers specific capacity of 740 mA·h·g−1 at a current density of 0.1 A·g−1. After 40 cycles at this current density the material still reached a capacity retention of 91%. Our findings show that this composite material could find application in electrochemical energy storage and generation devices where high flexibility and mechanical strength are desired.
  • 机译 通过叶酸的受控磷酸处理合成用于氧还原反应的P和N掺杂碳催化剂
    摘要:Herein, we synthesized P- and N-doped carbon materials (PN-doped carbon materials) through controlled phosphoric acid treatment (CPAT) of folic acid (FA) and probed their ability to catalyze the oxygen reduction reaction (ORR) at the cathode of a fuel cell. Precursors obtained by heating FA in the presence of phosphoric acid at temperatures of 400–1000 °C were further annealed at 1000 °C to afford PN-doped carbon materials. The extent of precursor P doping was maximized at 700 °C, and the use of higher temperatures resulted in activation and increased porosity rather than in increased P content. The P/C atomic ratios of PN-doped carbon materials correlated well with those of the precursors, which indicated that CPAT is well suited for the preparation of PN-doped carbon materials. The carbon material prepared using a CPAT temperature of 700 °C exhibited the highest ORR activity and was shown to contain –C–PO2 and –C–PO3 moieties as the major P species and pyridinic N as the major N species. Moreover, no N–P bonds were detected. It was concluded that the presence of –C–PO2 and –C–PO3 units decreases the work function and thus raises the Fermi level above the standard O2/H2O reduction potential, which resulted in enhanced ORR activity. Finally, CPAT was concluded to be applicable to the synthesis of PN-doped carbon materials from N-containing organic compounds other than FA.

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