Metal-organic frameworks (MOFs)-based photocatalysis technology has great potential to degrade or even completely mineralize organic pollutants. UiO-66, one of the typical MOFs, attracted extensive attentions and exhibits spatially low valence band position to induce strong oxidizing holes for mineralization of pollutants. However, severe carrier recombination limits their photocatalytic performance. Herein, we have designed an 3D/2D MOF/MXene heterojunction photocatalyst using UIO-66 as the prototype, in which octahedral UIO-66 were evenly dispersed on 2D MXene nanosheets, significantly improves the carrier separation kinetics for complete pollutants mineralization. Series characterizations of time-resolved photoluminescence (TRPL), Transient surface photovoltage spectrum (TPV), and in situ XPS spectra show that the binding of UIO-66 to MXene induces directional transport of photogenerated carriers in UIO-66, in which electrons migrate to the surface of 2D MXene and strong oxidizing holes remain over UIO-66. Therefore, the carrier lifetime of the UIO-66/MXene heterojunction (5.33 ns) is 2.5 times that of the pure UIO-66 (2.13 ns). As a proof of concept, the degradation efficiencies of series stubborn pollutants reach above 99.3 % within 90 min, especially the mineralization rate close to 100 %, superior than most previously reported works.
Anion-exchange membrane water electrolysis (AEMWE) represents a prospective technology for hydrogen production but suffers from the lack of efficient oxygen evolution electrocatalysts with high activity, robust stability, and reduced cost. Herein, we report pyrochlore-type bismuth ruthenates (Bi 2 Ru 2 O 7 , BRO) as promising electrocatalysts for oxygen evolution reaction (OER), which exhibits more than 20 times higher OER activity than RuO 2 yet with 48.3 wt.% less Ru content. The high intrinsic activity of BRO originates from the regulated local electronic structure of Ru sites by Bi, optimizing the adsorption behavior of oxygen intermediates and thus boosting the OER kinetics. Moreover, the assembled AEM electrolyzer with BRO as the anode can show a higher energy saving efficiency and a slower activity decay over a 120-h continuous operation in comparison to RuO 2 electrolyzer.
Parkinson's disease (PD) is a neurodegenerative condition marked by a steady loss of dopaminergic neurons in the brain's substantia nigra. Prompt identification and tracking of PD progression are essential for prompt intervention and efficient PD care. In this study, we developed an immunofluorescence detection approach for alpha-synuclein (alpha-syn), a critical biomarker associated with PD, that is both extremely sensitive and specific. Using polyethylene glycol (PEG)-functionalized magnetic beads (MBs) and an Ag+ fluorescence probe (Ag+-FP) based on Rhodamine 6 G, the suggested method makes use of an immunofluorescence detection system. The system's workings are based on antigen-antibody complexes. Identified as Ab1-MBs@alpha-syn@Ab2-Ag NPs, the immunocomplexes encapsulate alpha-synuclein between anti-alpha-synuclein antibodies (Ab1) fixed on amino-MBs and Ag Nanoparticles functionalized with matching Ab2. alpha-synuclein detection was accomplished at a limit of less than 8 pg/mL through optimization of pH, reaction duration, and antibody concentration. The method showed very little cross-reactivity with other widely used biomarkers and a high specificity. The system showed a linear range of 524.8 ng/mL to 0.2 ng/mL. The results, which showed recovery values ranging from 97.00 % to 99.57 % and were consistent with those obtained using a commercial ELISA kit, indicated the system's potential for clinical applications in the diagnosis and monitoring of PD.
Near-infrared light occupies 54.3% of the solar spectrum and has greater penetration depth, and its effective utilization is of great significance in the practical application of photocatalysis on a larger scale. However, the development of catalysts that can directly utilize near-infrared light is still a huge challenge. This paper proposes a strategy to directly utilize near-infrared light (excitation wavelength extending to 850 nm) by creating carbon material doped with a high-spin-state Co(II)-N x single-atom site. In the near-infrared-light-irradiated photooxidation of 1,5-dihydroxynaphthalene, the yield of juglone can reach 45% without a significant decrease, even when the catalytic volume is increased by 20 times, which was much higher than that irradiated by 460 nm wavelength (reduced by about 23%). Our study sets the stage for fabricating stable NIR photocatalysts and provides a solution to directly enhance NIR photooxidation in a large-scale manner.
MoSi2N4 is an emergent two-dimensional(2D)material,which has received much attention because of its excellent performance over semiconductors,including excellent environmental stability and high carrier mobility.However,the formation of intrinsic defects in semiconductors is often inevitable and can significantly affect device performance.By using density functional theory(DFT),we analyze the properties and effects of intrinsic point defects in MoSi2N4.We first confirm the consistency of our results with current experimental data.After that,the formation energy values of twelve native defects reveal that the antisite defect of molybdenum substituting for silicon(MoSi)defect dominates in all intrinsic defects.Under the constraint of overall charge neutrality,self-consistent Fermi level calculations reveal that MoSi2N4 with only intrinsic defects exhibits intrinsic characteristics,highlighting its potential as a semiconductor device material.However,this intrinsic nature contradicts the p-type characteristics observed in two-dimensional MoSi2N4.In the subsequent defect concentrations,we find that both n-type and p-type behavior can be easily realized by doping appropriate impurities without being compensated by native defects.This suggests that the p-type characteristics of MoSi2N4 during growth may result from p-type impurities introduced under non-equilibrium growth conditions or silicon vacancy defects.Our findings not only demonstrate the potential applications of MoSi2N4 in semiconductor devices but also provide valuable guidance for future studying the defect mechanisms of this material.
The Ag ions with the same fluence and different energies as well as the Au ions with the same energy and different fluences were separately implanted into SiO2 wafers to prepare Ag-E30, Ag-E40, Ag-E50, Au-F6.0, Au-F4.5, and Au-F3.0 samples as the candidates for the localized surface plasmon resonance sensor. The prepared samples' structural and optical properties were studied in depth. The results revealed that among Ag-E30, Ag-E40, and Ag-E50 samples, Ag-E40 sample had a single nanocomposite surface layer, and its characteristic reflection peak linearly depended in position on the refractive index of overlay owing to the stronger interparticle interaction. For Au-F6.0, Au-F4.5, and Au-F3.0 samples, they all featured a single nanocomposite surface layer and showed a linear dependence of the characteristic reflection peak's position and the overlay's refractive index. Considering the cost of preparation, Au-F3.0 sample should be an optimal sensor although its refractive index sensitivity was slightly smaller.
Using 0.5-mm-thick SiO2 wafers as substrates, Au3+Ag3 sample was prepared by sequentially implanting 45 keV Au ions and 30 keV Ag ions to the same fluence of 3.0 x 10(16) ions/cm(2), and Zn2+Au4.5 sample was fabricated by first implanting 40 keV Zn ions to a fluence of 2.0 x 10(16) ions/cm(2) and then 30 keV Au ions to a fluence of 4.5 x 10(16) ions/cm(2). The structural and optical properties of the two samples as well as their refractive index sensitivities were systematically investigated. The results revealed that although Au3+Ag3 sample did not possess a single nanocomposite surface layer due to the formation of approximately double-layer Au-Ag alloy nanoparticles with minor difference in composition, it still had a chance to become a refractive index sensor since its characteristic reflection signal associated with the shallower-layer Au-Ag alloy nanoparticles linearly depended on the refractive index of the monitored medium in terms of intensity. In Zn2+Au4.5 sample, a single nanocomposite surface layer containing Au nanoparticles was formed. Owing to the presence of Zn2SiO4, the dielectric environment of Au nanoparticles was slightly improved. As a result, the Zn2+Au4.5 sample, compared to that implanted with Au ions alone, increased by similar to 32% in refractive index sensitivity.
This study introduces a novel sol-gel synthesis route that combines the metal alkoxide and nonalkoxide methods to synthesize highly preferentially oriented potassium sodium niobate (KNN) films. In this approach, C10H25NbO5 and Nb2O5 are used as niobium sources to synthesize KNN sols, which are then alternately spin-coated to form the desired KNN film (referred to as e-KNN/o-KNN). Pure C10H25NbO5 source KNN film (e-KNN) and pure Nb2O5 source KNN film (o-KNN) are also synthesized as control samples. As expected, alternating spin-coating facilitates the enhancement of (h00)-preferred orientation and crystallinity, and both were superior to the KNN film with alternating e-KNN and o-KNN layers compared with the two pure KNN films. Interestingly, variations in annealing temperature do not affect the crystalline characteristics of these three types of KNN films, indicating that the synthesis route plays a predominant role in determining the microstructural characteristics. Furthermore, the dielectric response and optical properties of KNN films can also be precisely tailored through the synthesis route. For instance, using Nb2O5 as a niobium source can significantly enhance the dielectric constant of KNN films, whereas substituting C10H25NbO5 for Nb2O5 can effectively accelerate the dielectric polarization speed of KNN films, thereby reducing their high-frequency dielectric losses. This research provides new insights and significant guidance for tailoring the sol-gel synthesis, microstructural characteristics, and performance of KNN films. [GRAPHICS] .
The development of electrocatalysts for the oxygen evolution reaction (OER) especially in acidic media remains the major challenge that still requires significant advances, both in material design and mechanistic exploration. In this study, the incorporation of cobalt in Y 2‐x Co x Ru 2 O 7−δ results in an ultrahigh OER activity because of the charge redistribution at e g orbitals between Ru and Co atoms. The Y1. 75 Co 0.25 Ru 2 O 7−δ electrocatalyst exhibits an extremely small overpotential of 275 mV in 0.5 m H 2 SO 4 at the current density of 10 mA cm −2 , which is smaller than that of parent Y 2 Ru 2 O 7−δ (360 mV) and commercial RuO 2 (286 mV) catalysts. The systematic investigation of the composition related to OER activity shows that the Co substitution will also bring other effective changes, such as reducing the bandgap, and creating oxygen vacancies, which result in fast OER charge transfer. Meanwhile, the strengthening of the bond hybridization between the d orbitals of metal (Y and Ru) and the 2p orbitals of O will intrinsically enhance the chemical stability. Finally, theoretical calculations indicate that cobalt substitution reduces the theoretical overpotential both through an adsorbate evolution mechanism and a lattice oxygen‐mediated mechanism.
The development of highly active catalysts for eliminating volatile organic compounds (VOCs) at low temperature is desirable but remains challenging. In this study, a series of Ag-loaded MnCeO x catalysts were fabricated. Catalysts with an Ag loading of 5 wt.% exhibited the highest catalytic activity (T 90 = 242 °C) and excellent stability in H 2 O, NO 2 , and CO atmosphere. Characterization results revealed that the introduction of Ag increased Mn 4+ and Ce 3+ concentrations and enhanced surface oxygen migration capability, which is conducive to the adsorption and dissociation of propane and O 2 . Combining in-situ diffuse reflectance infrared Fourier transform and discrete Fourier transform calculation revealed a novel propane oxidation pathway on MnCeO x and Ag/MnCeO x . The addition of Ag species can convert propane into propylene in the initial stage and reduce the activation energy . This study supplied a novel insight into Ag-doped catalysts catalytic mechanism for VOCs oxidation reaction.
1D van der Waals (vdW) materials have attracted significant interest in recent years due to their giant anisotropic and weak interlayer-coupled characters. More 1D vdW materials are urgently to be exploited for satisfying the practice requirement. Herein, the study of 1D vdW ternary HfSnS3 high-quality single crystals grown via the chemical vapor transport technique is reported. The Raman vibration modes and band structure of HfSnS3 are analyzed via DFT calculations. Its strong in-plane anisotropic is verified by the polarized Raman spectroscopy. The field-effect transistors (FETs) based on the HfSnS3 nanowires demonstrate p-type semiconducting behavior as well as outstanding photoresponse in a broadband range from UV to near-infrared (NIR) with short response times of ≈0.355 ms, high responsivity of ≈11.5 A W-1 , detectivity of ≈8.2 × 1011 , external quantum efficiency of 2739%, excellent environmental stability, and repeatability. Furthermore, a typical photoconductivity effect of the photodetector is illustrated. These comprehensive characteristics can promote the application of the p-type 1D vdW material HfSnS3 in optoelectronics.
Au/SiO2 nanocomposite refractive index sensitive element was prepared by implanting 30 keV Au ions into a 0.5 -mm-thick SiO2 wafer at a fluence of 4.5 x 1016 ions/cm2. Combining this sensitive element with other com-ponents, a device was built to measure the reflection spectra of water and 4 % brine in real time during the cooling courses. With the recorded characteristic reflection peaks' positions, two media's refractive indices were calculated, and their phase transition processes were discussed. The results revealed that the water-ice phase transition in the cooled water was a very fast process, and the water freezing and the progressive salt precipi-tation existed in the cooled brine. These satisfactory and reproducible results demonstrated that the ion-beam -synthesized Au/SiO2 nanocomposite refractive index sensitive element was quite stable in structure, and thus, it could find its niche in the fields of selecting phase transition materials, preserving biological cells, and desalinating frozen seawater, etc.
To better understand and utilize the optical reflection behaviors of the nanostructured materials containing small metal nanoparticles (NPs), we once proposed a hypothesis that the recorded characteristic reflection peak should originate from the competition between the localized surface plasmon resonance (LSPR) scattering and absorption of metal NPs. To prove our hypothesis, the Ag- and Au-ion-implanted samples are prepared again by separately introducing 30 keV Ag and Au ions into 0.5-mm-thick SiO 2 wafers to a fluence of 6 × 10 16 ions/cm 2 . Especially, the Au-ion-implanted sample is further annealed in flowing nitrogen at different temperatures. Then, using a transmission electron microscope and a fiber spectrometer, all samples’ cross-sectional observations and spectral measurements are conducted, respectively. Based on the consistency in peak position and the difference in wavelength range of the absorption and reflection light fields measured from the Ag-ion-implanted sample, the LSPR scattering and absorption of Ag NPs are demonstrated to be coexistent, and their competition are testified to be inevitable and achievable via a filtration process. Besides these indirect evidences for our hypothesis, a direct evidence is also found, which is the blueshift shown by the characteristic reflection peak observed from the rear surface of the Au-ion-implanted sample after annealing.
The monoclinic and hexagonal gallium tellurides (m-GaTe and h-GaTe) show different applications in optoelectronic devices. Compared to the m-GaTe, the h-GaTe is a metastable phase, which generally exists in ultrathin samples and is difficult to obtain by direct chemical reaction. Herein, a hexagonal ZnO-induced crystal growth strategy was used for the design and fabrication of h-GaTe. The high-quality h-GaTe nanosheets were successfully grown on the (001) surface of hexagonal ZnO by the chemical vapor deposition method under ambient pressure. The SEM, XPS, XRD, and HRTEM characterizations uncovered a flower-like nanosheet morphology and a hexagonal crystal structure for the obtained GaTe samples. Meanwhile, the conductive atomic force microscope measurement indicates that the obtained h-GaTe nanosheet is a p-type semiconductor. Based on the electron localization function simulation, the lattice-induced crystal growth of h-GaTe was demonstrated. The results give an insight into the synthesis of metastable phase crystal and open an avenue for fabricating new two-dimensional devices by p-type h-GaTe.
Magnesium (Mg) and its alloys are promising materials in the industrial and biomedical field, but the excessive corrosion rate limits their practical application. To improve the anti-corrosion property of Mg alloys, the composite coating composed of calcium phosphate (CaP) and chitosan (CS) was prepared on AZ31 Mg alloy via simple electrophoretic deposition and chemical conversion method. The water contact angle (WCA) of the composite coating was as high as 158.6° after being modified by stearic acid. Furthermore, a superhydrophobic single CaP coating with the WCA value of 158.5° was fabricated by a chemical conversion method and low energy modification. The superhydrophobic coatings exhibited good self-cleaning properties to prevent the pollution of different pollutants. Furthermore, the obtained superhydrophobic Ca-P/CS composite coating can withstand more times of tape-peeling because of its better bonding ability. Moreover, compared with the superhydrophobic single CaP coating, the composite coating can provide more effective protection to the AZ31 substrate in electrochemical measurements and immersion test. Therefore, the superhydrophobic Ca-P/CS composite coating with significant performance advantages can expand the application fields of Mg alloys.
This paper employs the isothermal compression method to study the forging process of new aluminum alloy and analyzes its law of thermal deformation behavior at the temperature of 400~550°C and the strain rate of 1~-10-3s-1. It is found that flow stress is correlated with the temperature and strain rate and that the stress level decreases with the increase of temperature and the decrease of strain rate. This reveals the evolution law of the microstructure of the aluminum alloy in thermal deformation and lays a foundation for the subsequent studies and optimizationof the forging process.
Ag/SiO2 and Au/SiO2 samples were prepared by separately implanting 30 keV Ag and Au ions into 0.5-mm-thick SiO2 slabs at a fluence of 6 x 10(16) ion center dot cm(-2), and their optical and structural properties were studied in detail by using a fiber spectrometer and a transmission electron microscope, respectively. Our results showed that the two samples featured by their respective nanocomposite surface layers were asymmetrical in structure, and hence, their characteristic signals in the reflectance spectra excited by the lights incident from the rear surfaces were able to exhibit corresponding blueshifts when the overlays on the implanted surfaces were increased in refractive index with respect to air. Our results also showed that each of characteristic signals was strongly dependent on the localized surface plasmon resonance (LSPR) behavior of the involved Ag or Au nanoparticles (NPs), and it could not appear at a wavelength position smaller than or equal to that of the LSPR absorption peak since the involved Ag or Au NPs were quite small in size. These results meant that the two samples could be regarded as the LSPR sensors with a negative refractive index sensitivity (RIS), although their sensing abilities would lose when the overlays were very large in refractive index. Especially, the two samples were demonstrated to be relatively high in stability because the involved Ag and Au NPs were closely hugged and chemically protected by the matrices of SiO2, and consequently, they could have a chance to become prospective sensing devices in some special fields as long as their RISs and linearities could be improved in the future. The above findings substantially confirmed that the metal ion implantation into transparent dielectric slab was an effective route to the high-stability LSPR sensors.
Gahnite (ZnAl2O4) is widely used in different fields including optics and catalysis, but is rarely used as the superhydrophobic material. Thermal decomposition of layered double hydroxide (LDH) materials is a way to prepare gahnite materials. In this paper, a Zn-Al LDH coating in-situ grown on aluminum alloy 6061 was used as the precursor, and a gahnite superhydrophobic coating was fabricated by calcination and stearic acid modification. The effects of calcination temperature and calcination time on the wettability and microstructure of the gahnite coating were investigated. It showed that a micro-sheet structure attached by nanoneedle was constructed after calcining the Zn-Al LDH coating at 500 degrees C for 2 h. After modification, the stearic acid molecules were stored on the coating due to the chemical bonding and adsorption, obtaining a superhydrophobic surface with the average contact angle of 158.8 degrees and the sliding angle less than 2 degrees. Compared with the Zn-Al LDH superhydrophobic coating without calcination, the stability in mechanical damage, high-temperature environment, and different chemical solutions of gahnite superhydrophobic coating was obviously improved. Furthermore, after chemical damage or contamination, the superhydrophobic property of the gahnite coating could be self-healing by external high-temperature stimulati.
Frequent oil leakages and ever-increasing oily sewage have brought about serious damage to the ecological balance and human health. Therefore, effective and durable separation strategies and use of effective materials are highly desirable. In this work, a superwetting Ni3S2 coating was fabricated on stainless steel mesh (SSM) to achieve continuous oil/water separation. This mesh was superoleophilic in air but superhydrophobic and superoleophobic under oil and water. Once immersed in a liquid, oil/water droplets displayed large contact angles and lower adhesion. A bidirectional T-tube device integrated with two meshes at the two exit ends with inverse wettability was employed to separate oil/water mixtures. This system displayed high separation efficiencies and flux regardless of the oil density, and the separation efficiency was largely maintained after 100 cycles of separation. The same device could also separate immiscible organic solvents. Moreover, the Ni3S2@SSM showed photocatalysis to degrade water-soluble dyes targeting to further relief the water pollution. This multi-superwetting Ni3S2@SSM is expected to be a promising material for practical oil/water separation.