Single-Pixel Imaging Based on Deep Learning Enhanced Singular Value Decomposition.

We propose and demonstrate a single-pixel imaging method based on deep learning network enhanced singular value decomposition. The theoretical framework and the experimental implementation are elaborated and compared with the conventional methods based on Hadamard patterns or deep convolutional autoencoder network. Simulation and experimental results show that the proposed approach is capable of reconstructing images with better quality especially under a low sampling ratio down to 3.12%, or with fewer measurements or shorter acquisition time if the image quality is given. We further demonstrate that it has better anti-noise performance by introducing noises in the SPI systems, and we show that it has better generalizability by applying the systems to targets outside the training dataset. We expect that the developed method will find potential applications based on single-pixel imaging beyond the visible regime.

High-efficiency terahertz single-pixel imaging based on a physics-enhanced network.

As an alternative solution to the lack of cost-effective multipixel terahertz cameras, terahertz single-pixel imaging that is free from pixel-by-pixel mechanical scanning has been attracting increasing attention. Such a technique relies on illuminating the object with a series of spatial light patterns and recording with a single-pixel detector for each one of them. This leads to a trade-off between the acquisition time and the image quality, hindering practical applications. Here, we tackle this challenge and demonstrate high-efficiency terahertz single-pixel imaging based on physically enhanced deep learning networks for both pattern generation and image reconstruction. Simulation and experimental results show that this strategy is much more efficient than the classical terahertz single-pixel imaging methods based on Hadamard or Fourier patterns, and can reconstruct high-quality terahertz images with a significantly reduced number of measurements, corresponding to an ultra-low sampling ratio down to 1.56%. The efficiency, robustness and generalization of the developed approach are also experimentally validated using different types of objects and different image resolutions, and clear image reconstruction with a low sampling ratio of 3.12% is demonstrated. The developed method speeds up the terahertz single-pixel imaging while reserving high image quality, and advances its real-time applications in security, industry, and scientific research.

Droplet manipulation with polarity-dependent low-voltage electrowetting on an open slippery liquid infused porous surface.

This paper reports an open-loop method for highly efficient and precise droplet manipulation with polarity-dependent low-voltage electrowetting on a perfluorinated silane modified slippery liquid infused porous surface (SLIPS) in which a droplet can be driven between individual square electrodes. The electrowetting phenomenon on modified SLIPS was investigated first, and it exhibited an up to 55° contact angle difference with respect to voltage polarity while the threshold voltage was reduced to only 2 V. Then, a coplanar electrode experiment was designed to study the performance of droplet manipulation on several modified SLIPS samples with different vertically placed times and silicon oil viscosities. The optimal condition for preparing a modified SLIPS membrane is that a sample is placed vertically for 2 hours after infusing 10 cSt silicon oil, on which the droplet can be driven with the fastest velocity, and the activation voltage for moving a droplet is only 8 V. Finally, multi-droplet simultaneous and continuous manipulation on modified SLIPS in bi-direction on a loop of square electrodes was achieved. Interestingly, unlike asymmetric electrowetting, actuation methods on a solid insulator and hydrophobic layers, the droplet actuation velocity was not limited by the contact angle saturation effect and always increased with the applied voltage on modified SLIPS. This method achieves a very wide range of droplet continuous manipulation velocities from 0.075 mm s-1 to 123 mm s-1 under 20 V to 500 V applied voltage and the continuous droplet actuation voltage exhibits at least a 15-fold decrease compared to that of an unmodified SLIPS membrane.

Nanoconfined Ionic Liquids.

Ionic liquids (ILs) have been widely investigated as novel solvents, electrolytes, and soft functional materials. Nevertheless, the widespread applications of ILs in most cases have been hampered by their liquid state. The confinement of ILs into nanoporous hosts is a simple but versatile strategy to overcome this problem. Nanoconfined ILs constitute a new class of composites with the intrinsic chemistries of ILs and the original functions of solid matrices. The interplay between these two components, particularly the confinement effect and the interactions between ILs and pore walls, further endows ILs with significantly distinct physicochemical properties in the restricted space compared to the corresponding bulk systems. The aim of this article is to provide a comprehensive review of nanoconfined ILs. After a brief introduction of bulk ILs, the synthetic strategies and investigation methods for nanoconfined ILs are documented. The local structure and physicochemical properties of ILs in diverse porous hosts are summarized in the next sections. The final section highlights the potential applications of nanoconfined ILs in diverse fields, including catalysis, gas capture and separation, ionogels, supercapacitors, carbonization, and lubrication. Further research directions and perspectives on this topic are also provided in the conclusion.

CO tolerance of Pt/FeOx catalyst in both thermal catalytic H2 oxidation and electrochemical CO oxidation: the effect of Pt deficit electron state.

CO poisoning of Pt catalysts is one of the major challenges to the commercialization of proton exchange membrane fuel cells. One promising solution is to develop CO-tolerant Pt-based catalysts. A facilely synthesized Pt/FeOx catalyst exhibited outstanding CO tolerance in the oxidation of H2 and electrochemical CO stripping. Light-off temperature of H2O formation over Pt/FeOx was achieved even below 30 °C in the presence of 3000 ppm CO at a space velocity of 18 000 mL g-1cat h-1. For the electrochemical oxidation of CO, the onset and peak potentials decreased by 0.17 V and 0.10 V, respectively, in comparison with those of commercial Pt/C. More importantly, by a combination of hard X-ray photoemission spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies it was found that the decreased electron density of Pt in Pt/FeOx enhanced the mobility of adsorbed CO, suppressed Pt-CO bonding and significantly increased the CO tolerance of Pt/FeOx.

Ionic-liquid-based dispersive liquid-liquid microextraction coupled with high-performance liquid chromatography for the forensic determination of methamphetamine in human urine.

Determination of methamphetamine in forensic laboratories is a major issue due to its health and social harm. In this work, a simple, sensitive, and environmentally friendly method based on ionic liquid dispersive liquid-liquid microextraction combined with high-performance liquid chromatography was established for the analysis of methamphetamine in human urine. 1-Octyl-3-methylimidazolium hexafluorophosphate with the help of disperser solvent methanol was selected as the microextraction solvent in this process. Various parameters affecting the extraction efficiency of methamphetamine were investigated systemically, including extraction solvent and its volume, disperser solvent and its volume, sample pH, extraction temperature, and centrifugal time. Under the optimized conditions, a good linearity was obtained in the concentration range of 10-1000 ng/mL with determination coefficient >0.99. The limit of detection calculated at a signal-to-noise ratio of 3 was 1.7 ng/mL and the relative standard deviations for six replicate experiments at three different concentration levels of 100, 500, and 1000 ng/mL were 6.4, 4.5, and 4.7%, respectively. Meanwhile, up to 220-fold enrichment factor of methamphetamine and acceptable extraction recovery (>80.0%) could be achieved. Furthermore, this method has been successfully employed for the sensitive detection of a urine sample from a suspected drug abuser.

Development of a general non-noble metal catalyst for the benign amination of alcohols with amines and ammonia.

The N-alkylation of amines or ammonia with alcohols is a valuable route for the synthesis of N-alkyl amines. However, as a potentially clean and economic choice for N-alkyl amine synthesis, non-noble metal catalysts with high activity and good selectivity are rarely reported. Normally, they are severely limited due to low activity and poor generality. Herein, a simple NiCuFeOx catalyst was designed and prepared for the N-alkylation of ammonia or amines with alcohol or primary amines. N-alkyl amines with various structures were successfully synthesized in moderate to excellent yields in the absence of organic ligands and bases. Typically, primary amines could be efficiently transformed into secondary amines and N-heterocyclic compounds, and secondary amines could be N-alkylated to synthesize tertiary amines. Note that primary and secondary amines could be produced through a one-pot reaction of ammonia and alcohols. In addition to excellent catalytic performance, the catalyst itself possesses outstanding superiority, that is, it is air and moisture stable. Moreover, the magnetic property of this catalyst makes it easily separable from the reaction mixture and it could be recovered and reused for several runs without obvious deactivation.

Intrinsic electric fields in ionic liquids determined by vibrational Stark effect spectroscopy and molecular dynamics simulation.

The electric fields of ionic liquids are only slightly higher than those of common molecular solvents, and are strongly structure-dependent; they noticeably decrease with anion size because of increased separation of ions, and slightly decrease as the alkyl chain elongates due to increasing spatial heterogeneity. These were the key results of vibrational Stark effect spectroscopy and molecular dynamics simulations.

Sonochemical formation of iron oxide nanoparticles in ionic liquids for magnetic liquid marble.

Ionic liquids (ILs)-stabilized iron oxide (Fe(2)O(3)) nanoparticles were synthesized by the ultrasonic decomposition of iron carbonyl precursors in [EMIm][BF(4)] without any stabilizing or capping agents. The Fe(2)O(3) nanoparticles were isolated and characterized by X-ray powder diffraction, transmission electron microscopy and susceptibility measurements. The physicochemical properties of ILs containing magnetic Fe(2)O(3) nanoparticles (denoted as Fe(2)O(3)@[EMIm][BF(4)]), including surface properties, density, viscosity and stability, were investigated in detail and compared with that of [EMIm][BF(4)]. The Fe(2)O(3)@[EMIm][BF(4)] can be directly used as magnetic ionic liquid marble by coating with hydrophobic and unreactive polytetrafluoroethylene (PTFE), for which the effective surface tension was determined by the puddle height method. The resulting magnetic ionic liquid marble can be transported under external magnetic actuation, without detachment of magnetic particles from the marble surface that is usually observed in water marble.

Organic ligand-free alkylation of amines, carboxamides, sulfonamides, and ketones by using alcohols catalyzed by heterogeneous Ag/Mo oxides.

Complicated and expensive organic ligands are normally essential in fine chemical synthesis at preparative or industrial levels. The synthesis of fine chemicals by using heterogeneous catalyst systems without additive organic ligand is highly desirable but severely limited due to their poor generality and rigorous reaction conditions. Here, we show the results of carbon-nitrogen or carbon-carbon bond formation catalyzed by an Ag/Mo hybrid material with specific Ag(6) Mo(10) O(33) crystal structure. 48 nitrogen- or oxygen-containing compounds, that is, amines, carboxamides, sulfonamides, and ketones, were successfully synthesized through a borrowing-hydrogen mechanism. Up to 99 % isolated yields were obtained under relatively mild conditions without additive organic ligand. The catalytic process shows promise for the efficient and economic synthesis of amine, carboxamide, sulfonamide, and ketone derivatives because of the simplicity of the system and ease of operation.

Ionic liquid-modified dyes and their sensing performance toward acids in aqueous and non-aqueous solutions.

Six ionic liquid (IL)-modified dyes were synthesized and characterized. Compared to the methyl red and methyl orange, these IL-modified [MR](-)- or [MO](-)-based dyes exhibit lower melting points and enhanced solubility, and can be used as sensitive indicators towards free proton in both aqueous and non-aqueous solutions. This work also supplies a new concept of developing novel modified materials with the ILs.

Nanocomposites of ionic liquids confined in mesoporous silica gels: preparation, characterization and performance.

A series of nanocomposites of ionic liquids (ILs) were prepared via a modified sol-gel method. The ILs were physically confined in mesoporous silica gels with 5-40% content. ILs from imidazolium, thiophenium and ammonium with different anions were prepared and used. Characterization using the Brunauer-Emmett-Teller (BET) method, Fourier transform infrared (FT-IR) spectroscopy, temperature-programmed desorption (TPD), differential scanning calorimetry (DSC), inverse gas chromatography (IGC), temperature-controlled Raman and fluorescence emission spectroscopies was conducted to explore any confinement effects. BET results showed that, depending on the ILs and their contents, the average pore diameter of the pure silica gel was 3-12 nm after the confined ILs were removed completely. It was suggested that ILs aggregated on the nanoscale in the mesoporous silica gel. In comparison with bulk ILs and ILs coated onto silica gels (IL/sg), IL nanocomposites (IL-sg) displayed remarkably low specific heat capacities (C(p) was in the range 0.3-1.2 J g(-1) K(-1)), disordered vibrational conformations (without phase transitions in the range -100-200 degrees C), greater interactions with hydrocarbon solutes (adsorption capacities of 0.3-0.4 g per 100 g for confined ILs with CO(2) gas), and greatly enhanced fluorescence emission (up to 200 times stronger than bulk ILs). Furthermore, Based on the specific solubility of different compounds, the nanocomposites could also be applied to the separation of CO(2) from CO(2)/N(2) mixtures and thiophene from thiophene/octane mixtures.

Novel cyclic sulfonium-based ionic liquids: synthesis, characterization, and physicochemical properties.

A new series of ionic liquids composed of three cyclic sulfonium cations and four anions has been synthesized and characterized. Their physicochemical properties, including their spectroscopic characteristics, ion cluster behavior, surface properties, phase transitions, thermal stability, density, viscosity, refractive index, tribological properties, ion conductivity, and electrochemical window have been comprehensively studied. Eight of these salts are liquids at room temperature, at which some salts based on [NO(3)](-) and [NTf(2)](-) ions exhibit organic plastic crystal behaviors, and all the saccharin-based salts display relatively high refractive indices (1.442-1.594). In addition, some ionic liquids with the [NTf(2)](-) ion exhibit peculiar spectroscopic characteristics in FTIR and UV/Vis regions, whilst those salts based on the [DCA](-) ion show lower viscosities (34.2-62.6 mPa s at 20 degrees C) and much higher conductivities (7.6-17.6 mS cm(-1) at 20 degrees C) than most traditional 1,3-dialkylimidazolium salts.

Photochromism of spiropyran in ionic liquids: enhanced fluorescence and delayed thermal reversion.

Photochromism of spiropyran and thermal reversion of MC in a series of imidazolium-based ionic liquids (ILs) were investigated via fluorescence and UV-vis absorption spectra. The fluorescence emission maxima (lambda(em)) of the colored merocyanine (MC) form is polarity dependent in all ILs and fluorescence intensity enhancement was first observed in ILs with respect to that observed in organic solvents (e.g., in [HOMIm][PF(6)], nearly 32-fold enhancement than ethanol). Moreover, the thermal decay of MC in all ILs is uniformly first order, and in comparison with polar solvents possessing comparable polarity (such as ethanol and acetonitrile), a significant retardation of the decay rate and increase of half-lifetime of MC form was observed, in particular at elevated temperature (e.g., at 313 K, MC decay with k of 5.19 x 10(-4) and 34.7 x 10(-4) s(-1) in [BMMIm][BF(4)] and ethanol, respectively). Abnormal thermodynamics of the thermal decay of MC in ILs were observed, activation energies in less polar ILs (88-97 kJ mol(-1)) have a larger value than in polar ILs (70-82 kJ mol(-1)), opposite that in organic solvents (70-80 kJ mol(-1) in nonpolar solvents and around 100 kJ mol(-1) in polar solvents), and all ILs exclusively exhibit minus activation entropies (-85.4 to -24.5 J K(-1) mol(-1)), similar to that of nonpolar solvents. Desolvation due to the conformational change during the thermal reversion between MC and the transition state may be the key to interpret this experimental result.

Novel chemoselective hydrogenation of aromatic nitro compounds over ferric hydroxide supported nanocluster gold in the presence of CO and H2O.

Chemoselective hydrogenation of aromatic nitro compounds were first efficiently achieved over Au/Fe(OH)(x) at 100-120 degrees C for 1.5-6 h (depending on different substrates) in the presence of CO and H(2)O.

Formation and Depolymerization of Oligomers during Thermal Cracking of Silicon-Containing Carbamates.

Polymerization reactions in the thermal cracking of N-substituted carbamates to produce the corresponding isocyanates significantly reduce the yield of isocyanates and thus vastly hinder the industrial application of such non-phosgene routes. Herein, we tried to recycle the oligomers generated during the thermal cracking of 3-ethylcarbamatopropyltriethoxysilane (CPTS) to produce 3-isocyanatopropyltriethoxysilane (IPTS). Firstly, the polymerized substrates of the pyrolysis reaction were analyzed by NMR, IR, MALDI-TOF-MS and TG, indicating the pyrolysis substrates were mixtures of CPTS (25 wt%), polyureas (74 wt%), imines, and other compounds (<1 wt %). The polyureas were generated by reaction of CPTS and IPTS. Then, the depolymerization of these polyureas was realized via alcoholysis in the presence of urea. It was found that the urea not only provides a carbonyl group source, but also forms hydrogen bonds with polyureas. In addition, NH3 co-produced can also modify the reaction system microenvironment, which might be favorable for the dissociation of polyureas. With optimized conditions, more than 96 % of polymerized substrates could be reverted to CPTS for secondary cracking.

Physicochemical properties of nitrile-functionalized ionic liquids.

A series of ionic liquids (ILs) based on nitrile-functionalized imidazolium, pyridinium, and quaternary ammonium as cations and chlorides and tetrafluoroborate, hexafluorophosphate, dicyanamide, and bis(trifluoromethanesulfonyl)imide as anions have been prepared and characterized. The physicochemical properties such as spectroscopic, thermal, solubility, surface, electrochemical, tribological, and toxic properties were comparatively studied. The results showed that the incorporation of a CN group to cations could result in remarkable changes in these properties. The reason resulting in such remarkable differences in the properties may be attributed to the conformational changes in the imidazolium groups caused by the interaction between the CN group with other neighboring cations or anions and the enhancement in hydrogen-bonding interactions due to the incorporation of a CN group.

Preparation of Carbon Nanotubes/Manganese Dioxide Composite Catalyst with Fewer Oxygen-Containing Groups for Li-O2 Batteries Using Polymerized Ionic Liquids as Sacrifice Agent.

Considering the significant influence of oxygen-containing groups on the surface of carbon involved electrodes, a carbon nanotube (CNT)-based MnO2 composite catalyst was synthesized following a facile method while using polymerized ionic liquids (PIL) as sacrifice agent. Herein, the PIL (polymerized hydrophobic 1-vinyl-3-ethylimidazolium bis ((trifluoromethyl)sulfonyl)imide) wrapped CNTs were prepared. The composite was applied to support MnO2 by the treatment of KMnO4 solution, taking advantage of the reaction between PIL and KMnO4, which excludes or suppresses the oxidation of CNTs, and the as-synthesized material with fewer oxygen-containing groups acted as a cathode catalyst for Li-O2 batteries, directly avoiding the application of binders. The catalyst shows enhanced activity compared to that of the samples without PIL, as verified by the lower overpotential during discharging and charging (0.97 V at the current density of 100 mA g-1). Meanwhile, the performance parameters such as Coulombic efficiency and rate capability were also improved for the Li-O2 battery utilizing this catalyst. Further, the formation of confined Li2O2 particles could be responsible for the reduction of charge potential of Li-O2 batteries due to the synergy effect of the intrinsic catalytic activity of MnO2 and fewer oxygen functional groups on the catalyst surface.