Rapid, sensitive, and selective detection of explosives such as 2,4,6-trinitrotoluene (TNT) and 2,4,6-trinitrophenol (TNP), especially using a facile paper sensor, is in high demand for homeland security and public safety. Although many strategies have been successfully developed for the detection of TNT, it is not easy to differentiate the influence from TNP. Also, few methods were demonstrated for the selective detection of TNP. In this work, via a facile and versatile method, 8-hydroxyquinoline aluminum (Alq(3))-based bluish green fluorescent composite nanospheres were successfully synthesized through self-assembly under vigorous stirring and ultrasonic treatment. These polymer-coated nanocomposites are not only water-stable but also highly luminescent. Based on the dramatic and selective fluorescence quenching of the nanocomposites via adding TNP into the aqueous solution, a sensitive and robust platform was developed for visual detection of TNP in the mixture of nitroaromatics including TNT, 2,4-dinitrotoluene (DNT), and nitrobenzene (NB). Meanwhile, the fluorescence intensity is proportional to the concentration of TNP in the range of 0.05-7.0 μg/mL with the 3σ limit of detection of 32.3 ng/mL. By handwriting or finger printing with TNP solution as ink on the filter paper soaked with the fluorescent nanocomposites, the bluish green fluorescence was instantly and dramatically quenched and the dark patterns were left on the paper. Therefore, a convenient and rapid paper sensor for TNP-selective detection was fabricated.
We developed a simple fabrication method to prepare a superamphiphobic aluminum surface. On the basis of a low-energy surface and the combination of micro- and nanoscale roughness, the resultant surface became super-repellent toward a wide range of liquids with surface tensions of 25.3-72.1 mN m(-1). The applied approach involved (1) the formation of an irregular microplateau structure on an aluminum surface, (2) the fabrication of a nanoplatelet structure, and (3) fluorination treatment. The chemical stability and mechanical durability of the superamphiphobic surface were evaluated in detail. The results demonstrated that the surface presented an excellent chemical stability toward cool corrosive liquids (HCl/NaOH solutions, 25 °C) and 98% concentrated sulfuric acid, hot liquids (water, HCl/NaOH solutions, 30-100 °C), solvent immersion, high temperature, and a long-term period. More importantly, the surface also exhibited robust mechanical durability and could withstand multiple-fold, finger-touch, intensive scratching by a sharp blade, ultrasonication treatment, boiling treatment in water and coffee, repeated peeling by adhesive tape, and even multiple abrasion tests under 500 g of force without losing superamphiphobicity. The as-prepared superamphiphobic surface was also demonstrated to have excellent corrosion resistance. This work provides a simple, cost-effective, and highly efficient method to fabricate a chemically stable and mechanically robust superamphiphobic aluminum surface, which can find important outdoor applications.
Direct visualization of spatiotemporal evolution of molecules and active sites during chemical transformation in individual catalyst crystal will accelerate the intuitive understanding of heterogeneous catalysis. So far, widespread imaging techniques can only provide limited information either with large probe molecules or in model catalyst of large size, which are beyond the interests of industrial catalysis. Herein, we demonstrate a feasible deep data approach via synergy of multiscale reaction-diffusion simulation and super-resolution structured illumination microscopy to illustrate the dynamical evolution of spatiotemporal distributions of gas molecules, carbonaceous species and acid sites in SAPO-34 zeolite crystals of several micrometers that are typically used in industrial methanol-to-olefins process. The profound insights into the inadequate utilization of activated acid sites and rapid deactivation are unveiled. The notable elucidation of molecular reaction-diffusion process at the scale of single catalyst crystal via this approach opens an interesting method for mechanism study in materials synthesis and catalysis.
In this study, a large-area superhydrophobic alumina surface with a series of superior properties was fabricated via an economical, simple, and highly effective one-step anodization process, and subsequently modified with low-surface-energy film. The effects of the anodization parameters including electrochemical anodization time, current density, and electrolyte temperature on surface morphology and surface wettability were investigated in detail. The hierarchical alumina pyramids-on-pores (HAPOP) rough structure which was produced quickly through the one-step anodization process together with a low-surface-energy film deposition [1H,1H,2H,2H-perfluorodecyltriethoxysilane (PDES) and stearic acid (STA)] confer excellent superhydrophobicity and an extremely low sliding angle. Both the PDES-modified superhydrophobic (PDES-MS) and the STA-modified superhydrophobic (STA-MS) surfaces present fascinating nonwetting and extremely slippery behaviors. The chemical stability and mechanical durability of the PDES-MS and STA-MS surfaces were evaluated and discussed. Compared with the STA-MS surface, the as-prepared PDES-MS surface possesses an amazing chemical stability which not only can repel cool liquids (water, HCl/NaOH solutions, around 25 °C), but also can show excellent resistance to a series of hot liquids (water, HCl/NaOH solutions, 30-100 °C) and hot beverages (coffee, milk, tea, 80 °C). Moreover, the PDES-MS surface also presents excellent stability toward immersion in various organic solvents, high temperature, and long time period. In particular, the PDES-MS surface achieves good mechanical durability which can withstand ultrasonication treatment, finger-touch, multiple fold, peeling by adhesive tape, and even abrasion test treatments without losing superhydrophobicity. The corrosion resistance and durability of the diverse-modified superhydrophobic surfaces were also examined. These fascinating performances makes the present method suitable for large-scale industrial fabrication of chemically stable and mechanically robust superhydrophobic surfaces.
Superlyophilic interfaces denote interfaces displaying strong affinity to diverse liquids, including superhydrophilic, superoleophilic, and superamphiphilic interfaces. When coming in contact with these interfaces, water or oil droplets tend to spread completely with contact angles close to 0°, presenting versatile applications including self‐cleaning, antifogging, controllable liquid transport, liquid separation, and so forth. Inspired by nature, scientists have developed various kinds of artificial superlyophilic (SLPL) interfaces in the past decades. In terms of dimensional characteristics, the artificial SLPL interfaces can be divided into four categories: i) 0D particles, whose dispersibility or catalytic performance can be notably enhanced by superlyophilicity; ii) 1D micro‐/nanofibers or nanotubes/channels, which can efficiently transfer liquids with SLPL interfaces; iii) 2D flat SLPL interfaces, on which different functional molecules can be deposited uniformly, forming ultrathin and smooth films; and iv) 3D structures, which can be obtained by either constructing 0D, 1D, or 2D SLPL materials separately or directly fabricating random SLPL frameworks, and can always be used as functional coatings or bulk materials. Here, natural and artificial SLPL interfaces are briefly introduced, followed by a short discussion of the limit between lyophilicity and lyophobicity, and then a snapshot of methods to generate SLPL interfaces is given. Specific focus is placed on recent achievements of constructing SLPL interfaces from zero to three dimensions. Following that, broad applications of SLPL interfaces in commercial areas will be introduced. Finally, a short summary and outlook for future challenges in this field is presented.
Mass transfer of guest molecules has a significant impact on the applications of nanoporous crystalline materials and particularly shape-selective catalysis over zeolites. Control of mass transfer to alter reaction over zeolites, however, remains an open challenge. Recent studies show that, in addition to intracrystalline diffusion, surface barriers represent another transport mechanism that may dominate the overall mass transport rate in zeolites. We demonstrate that the methanol-to-olefins (MTO) reaction can be modulated by regulating surface permeability in SAPO-34 zeolites with improved chemical liquid deposition and acid etching. Our results explicitly show that the reduction of surface barriers can prolong catalyst lifetime and promote light olefins selectivity, which opens a potential avenue for improving reaction performance by controlling the mass transport of guest molecules in zeolite catalysis.
Herein, the photophysical properties of two π-conjugated thienophenanthrene derivatives (6,9- and 5,10-DBTD) are reported. Their self-assembled monolayers in aliphatic hydrocarbon solvents under different concentrations were investigated by scanning tunneling microscopy on a graphite surface. The STM results revealed that the self-assembled structures of the two geometrical isomers exhibited absolutely different behaviors. At the aliphatic solvent/graphite interface, 6,9-DBTD produced almost a single stable coassembled linear structure, except for that with n-tridecane as the solvent. However, the self-assembly of 5,10-DBTD showed structural diversity, and it presented a gradient variety through increasing the chain length of the aliphatic solvents as well as the solution concentration. All ordered self-assembled adlayers critically depend on not only the interchain van der Waals (vdW) interactions, but also on multiple intermolecular interactions, including BrO[double bond, length as m-dash]C and BrS hetero-halogen bonds, homo-BrBr interactions, and HBr and HO hydrogen bonds. We proposed that the cooperation and competition of the intermolecular interactions involving a Br atom and interchain vdW forces induce this structural variety. Density functional theory calculations support to unravel the different elementary structural units based on halogen bonds and hydrogen bonds and were useful tools to dissect and explain the formation mechanism.
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