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Superhydrophobic materials have been widely applied in oil-water separation, self-cleaning, antifouling, and drag reduction; however, their role in liquid evaporation and drying remains unexplored. Inspired by the microstructure of the nonwetting legs of water striders, we designed a low-adhesion superhydrophobic cylindrical barrel (CB) derived from stainless-steel mesh (SSM) to enhance liquid thermal evaporation and drying. The CB was created by hydrothermally depositing zinc oxide (ZnO) with multilevel morphologies onto metal wires, followed by modification with low-surface-energy stearic acid (SA). We investigated the impact of the SSMCB on water evaporation and analyzed the decline in the liquid levels under varying porosities and temperatures through numerical normalization. A functional relationship was established between decline height, porosity, and temperature, revealing that the drop height increased from 3.7 to 25 mm as porosity increased from 0 to 0.5263. Moreover, the superhydrophobic coating demonstrated excellent resistance to friction and peeling, indicating improved mechanical stability.
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The direct catalytic asymmetric hydrogenation of pyridines for the synthesis of piperidines remains a challenge. Herein, we report a one-pot asymmetric hydrogenation of pyridines with subsequent N-alkylation using a traceless Brønsted acid activation strategy. Catalyzed by an iridium-BINAP complex, the substrates undergo ketone reduction, cyclization and pyridine hydrogenation in sequence to form indolizidines and quinolizidines. The absolute configuration of the stereocenter of the alcohol is retained and influences the formation of the second stereocenter. Experimental and theoretical mechanistic studies reveal that the chloride anion and certain noncovalent interactions govern the stereoselectivity of the cascade reaction throughout the catalytic process.
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Yellow-orange lights, valuable in photodynamic therapies, spectroscopy, and optogenetics, are limited by the narrow bandwidth and bulky setup via the conventional Raman or optical parametric oscillation processes. Moreover, flatness in the broad-band spectrum is also important for the aforementioned applications with extended functions. In this paper, by carefully designing grating-periods of a step-chirped PPMgLN ridge waveguide for sum frequency generation (SFG), we report a compact broad-band yellow-orange light with bandwidth of 5.6â nm and an un-reported flatness (<1.5â dB). Correspondingly, the optical conversion efficiency is 232.08%/W, which is the best SFG efficiency for PPMgLN at the yellow-orange region, to the best of our knowledge. The results could also be adopted for other broad-band SFG process toward the vis-infrared region in an integrated structure.
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We demonstrate a sub-nanosecond MOPA system with a pulse repetition frequency of 1 kHz at 1.06 µm, based on an integrated seed source with pulse energy of 6.2 mJ and two conductively cooled end-pumped Nd:YAG slab gain modules. After a 4-pass amplification stage and a double-pass amplification stage with amplification factors of 12.6 dB and 5.84 dB, respectively, maximum pulse energy of 434 mJ with pulse duration of 691 ps was obtained, corresponding to a peak power of 628 MW. Via adjusting the pump distribution to compensate the static wavefront distortion of the signal laser, the beam quality, at the maximum pulse energy, was optimized to be 2.5 mm·mrad and 2.2 mm·mrad respectively in the vertical and transverse directions. The results benefit a variety of applications including material processing, nonlinear frequency conversion, and lidars.
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Asymmetric reductive amination (ARA) is one of the most promising methods for the synthesis of chiral amines. Herein we report our efforts on merging two ARA reactions into a single-step transformation. Catalyzed by a complex formed from iridium and a steric hindered phosphoramidite, readily available and inexpensive aromatic ketones initially undergo the first ARA with ammonium acetate to afford primary amines, which serve as the amine sources for the second ARA, and finally provide the enantiopure C2 -symmetric secondary amine products. The developed process competently enables the successive coupling of inorganic and organic nitrogen sources with ketones in the same reaction system. The Brønsted acid additive plays multiple roles in this procedure: it accelerates the formation of imine intermediates, minimizes the inhibitory effect of N-containing species on the iridium catalyst, and reduces the primary amine side products.
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We evaluate the thermal effects of a c-cut Tm:YAP slab laser by considering the anisotropic properties of the biaxial YAP crystal. Significant improvements in thermal stress were demonstrated by selecting the crystallographic a-axis, which possesses higher thermal conductivity and thermal expansion, as the direction of the slab thickness. A maximum laser power of 30 W (E//a) at 2 µm was obtained under an incident LD power of 55 W with an optical conversion efficiency of 55.4% and slope efficiency of 61.8% using the a-slab. The slab laser was then used for realizing compact Ho lasers via intra-cavity pumping, resulting in a 0.8 W Ho:YAG laser and a 5.5 W Ho:YAP laser (E//b) at 2.12 µm and 2.13 µm, respectively.
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We develop a fluoride-based intra-cavity pumped Ho laser for the first time, where the severe thermal lensing of the intra-cavity pumping mechanism can be compensated by the negative thermal-optical property of the YLiF4 (YLF) host. A maximum output power of 11.3 W (π-pol) at 2062 nm, corresponding to a conversion efficiency of 28.2% from the incident diode laser to the Ho laser, was obtained with a power instability below 0.5% and a near diffraction limited beam quality with M2 of 1.06 and 1.25 in the horizontal and vertical directions, respectively. These are the maximum power and the best beam quality for the reported compact intra-cavity pumped Ho lasers, to the best of our knowledge.
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Classification of faults in mechanical components using machine learning is a hot topic in the field of science and engineering. Generally, every real-world running mechanical system exhibits personalized vibration behaviors that can be measured with acceleration sensors. However, faulty samples of such systems are difficult to obtain. Therefore, machine learning methods, such as support vector machine (SVM), neural network (NNs), etc., fail to obtain agreeable fault detection results through smart sensors. A personalized diagnosis fault method is proposed to activate the smart sensor networks using finite element method (FEM) simulations. The method includes three steps. Firstly, the cosine similarity updated FEM models with faults are constructed to obtain simulation signals (fault samples). Secondly, every simulation signal is separated into sub-signals to solve the time-domain indexes to generate the faulty training samples. Finally, the measured signals of unknown samples (testing samples) are inserted into the trained SVM to classify faults. The personalized diagnosis method is applied to detect bearing faults of a public bearing dataset. The classification accuracy ratios of six types of faults are 90% and 92.5%, 87.5% and 87.5%, 85%, and 82.5%, respectively. It confirms that the present personalized diagnosis method is effectiveness to detect faults in the absence of fault samples.
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We developed an 808 nm diode laser pumped composite Holmium laser via the integration of Tm-doped and Ho-doped YAG crystals into a single bulk structure. A maximum output power of 1.8 W at 2122 nm with near diffraction-limited beam quality was achieved for an absorbed pump power of approximately 7 W. Given that the pump wavelength is approximately 20 nm away from the absorption peak of the Tm-doped region of the crystal, pump wavelength adaptability of the Tm/Ho composite laser was effectively demonstrated. In this case, a pump range width in excess of 40 nm at approximately 800 nm was predicted by defining the pump spectrum of the gain medium. The temperature adaptability of the Ho laser was demonstrated by varying the cooling temperature from 9 °C to 27 °C. This resulted in Ho laser operation above 1.5 W with a power deviation below 10%. This work presents the experimental results for a compact assessable 2.1 µm laser without pump wavelength and operation temperature restrictions.
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We demonstrate an enhancement mechanism and thermal model for intra-cavity pumped lasers, where resonance enhancement in intra-cavity pumped Ho laser was achieved by manipulating the wavelength-drift nature of the Tm laser for the first time. Optical conversion efficiency of 37.5% from an absorbed 785 nm diode laser to a Ho laser was obtained with a maximum output power of 7.51 W at 2122 nm, which is comparable to the conversion efficiency in 1.9 µm LD pumped Ho lasers. Meanwhile, more severe thermal effects in the Ho-doped gain medium than the Tm-doped one at high power operation were verified based on the built thermal model. This work benefits the design or evaluation of intra-cavity pumped lasers, and the resonance enhancement originated from the difference in reabsorption loss between stark levels at the lasing manifolds of quasi-three-level rare-earth ions has great interest to improve the existing intra-cavity pumped lasers or explore novel lasers.
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We realize Ho laser operation in a composite Tm/Ho:YAG gain medium for the first time, to the best of our knowledge, which was integrated via diffusion bonding the Tm-doped and Ho-doped crystals into a single bulk structure. A maximum output power around 6 W was obtained with a slope efficiency of 40.1% and conversion efficiency (CE) of 33.6% from the absorbed 785 nm laser diode to 2122 nm Ho laser, which is comparable with CE in 1.9 µm LD pumped Ho lasers. Such a scheme is demonstrated to be another valid way for Ho laser generation here, which is of significance to be adopted in other host media or waveguide structures for an assessable, compact, and efficient Ho laser.
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We demonstrated a passively Q-switched solid-state Tm:YAG laser using topological insulator (TI) Bi2Te3 as the saturable absorber (SA) for the first time, to the best of our knowledge. The Q-switched laser pulses were obtained with the minimum pulse width of 382 ns, the maximum pulse energy of 4.8 µJ, the maximum average output power of 272 mW, and a pulse repetition rate of 57.67 kHz. The results indicate that Bi2Te3 can be a promising kind of saturable absorber in the 2 µm wavelength region.
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In this article we demonstrate how asymmetric total synthesis of (S)-rivastigmine has been achieved using direct asymmetric reductive amination as the key transformation in four steps. The route started with readily available and cheap m-hydroxyacetophenone, through esterification, asymmetric reductive amination, N-diphenylmethyl deprotection and reductive amination, to provide the final (S)-rivastigmine in 82% overall yield and 96% enantioselectivity. In the asymmetric reductive amination, catalysed by the iridiumâ»phosphoramidite ligand complex and helped by some additives, the readily prepared 3-acetylphenyl ethyl(methyl)carbamate directly reductively coupled with diphenylmethanamine to yield the chiral amine product in 96% ee and 93% yield.
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Rivastigmina/síntese química , Aminação , Avaliação Pré-Clínica de Medicamentos , Ligantes , Oxirredução , Rivastigmina/químicaRESUMO
We first demonstrate an efficient Ho:YAG laser intra-cavity pumped by a narrowband-diode-pumped Tm:YAG laser. The pump wavelength of the laser diode was selected according to the excitation peak which is also one of the absorption peaks of a 3.5 at. % Tm:YAG crystal and was locked by volume Bragg gratings. In the Tm laser experiment, a maximum output power of 11.12 W, corresponding to a slope efficiency of 51.6%, was obtained. In the Ho laser experiment, a maximum output power of 8.03 W at 2122 nm with a slope efficiency of 38% was obtained for 24.96 W of diode pump power incident on the Tm:YAG rod.
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The highly efficient and direct asymmetric reductive amination of arylacetones catalyzed by an iridium complex for the preparation of enantiomerically pure ß-arylamines is described. The monodentate phosphoramidite ligand exhibits superb reactivity (TONs of up to 20 000) and enantioselectivity (up to 99 % ee). Additives played important roles in this reductive coupling reaction.
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This report describes an additive-free iridium-catalyzed direct asymmetric reductive amination that enables the efficient synthesis of chiral ß-arylamines, which are important pharmacophores present in a wide variety of pharmaceutical drugs. The reaction makes use of bulky and tunable phosphoramidite ligands for high levels of enantiomeric control, even for alkylamino coupling partners which lack secondary coordinating sites. The synthetic value of this succinct procedure is demonstrated by single-step synthesis of multiple drugs, analogs and key intermediates. Mechanistic investigations reveal an enamine-reduction pathway, in which H-bonding, steric repulsion, and CH-π and electrostatic interactions play important roles in defining the spatial environment for the "outer-sphere" hydride addition.
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Exploring highly sensitive flexible electronic skins (e-skins) that can mimic the tactile and pain perception of human skin is an important prerequisite for achieving biomimetic robots and intelligent prosthetics. However, it is still difficult to realize both touch and pain sensing using a single pressure sensor. Herein, a novel flexible capacitive pressure sensor that can distinguish noxious pressure stimuli is proposed for detecting touch and pain, which is composed of a porous polydimethylsiloxane (PDMS) skeleton and a sodium alginate (SA) hydrogel core. The sensor employs two different working mechanisms depending on the range of external pressure, determining the mechanism of operation for transducing the sense of touch or pain. Such a unique structural design plays a crucial role in enhancing pain perception, leading to maximum sensitivity (14.25 kPa-1) in a large pressure regime (up to 400 kPa) and an adjustable pressure threshold. Moreover, the sensor also exhibits a fast response (45 ms) and recovery speed (70 ms), ensuring a sufficiently fast response to noxious pressure stimuli. Finally, we demonstrate the capabilities of a robotic hand based on the pressure sensor for precisely detecting both touch and pain, which shows great promise in developing intelligent robots and prosthetic limbs to prevent possible damage under external noxious stimuli.
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Alginatos , Dimetilpolisiloxanos , Hidrogéis , Pressão , Tato , Dimetilpolisiloxanos/química , Hidrogéis/química , Humanos , Porosidade , Alginatos/química , Dispositivos Eletrônicos Vestíveis , Dor/diagnóstico , Robótica/instrumentação , Capacitância ElétricaRESUMO
With the increasing use of plastic products globally, environmental pollution by plastic waste is becoming increasingly problematic. This study investigated the impacts of two types of polylactic acid microplastics, clear microplastics and aluminised film microplastics, on methane yield, microbial community, and volatile fatty acid accumulation during anaerobic co-digestion of cow manure and Chinese cabbage waste under different temperature conditions. The influence of the addition of air nanobubbles on microplastic degradation in the anaerobic digestion system we also examined. The results revealed that under thermophilic conditions, clear and aluminised film microplastics increased the methane yield, with the latter resulting in greater improvement. Conversely, under mesophilic conditions, the presence of microplastics reduced the methane yield, but the addition of Air-nanobubble partially mitigated this effect. Microplastics also affected the microbial community, with specific species showing correlations with methane yield. Methanothermobacter, which is linked to lactic acid conversion, was positively correlated with methane yield, whereas Methanomassiliicoccus levels increased in the presence of microplastics, particularly in the inhibited state of the digester. These results suggest that, under thermophilic conditions, microplastics may increase the cumulative methane yield by facilitating the degradation of lactic acid monomers. Furthermore, the aluminised film on microplastics could serve as an electrically conductive material during anaerobic digestion, potentially increasing the methane yield.
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A stable and seamless adhesion between the human skin and the hydrogel-based electronic skin is necessary for accurate sensing and human health monitoring in aquatic environments. Despite achieving significant progress in this field, it remains a great challenge to design skin-interfaced conductive hydrogels with high electrical conductivity, stablility, and seamless underwater adhesion to skin. Herein, a skin-inspired conductive multifunctional hydrogel is proposed, which has a wet-adhesive/hydrophilic and a non-adhesive/hydrophobic bilayer structure. The hydrogel shows high stretchability (â¼2400%) and an ultra-low modulus (4.5 kPa), which facilitate the conformal and seamless attachment of the hydrogel to the skin with reduced motion artifacts. Owing to synergistic physical and chemical interactions, this hydrogel can achieve reliable underwater adhesion and display remarkable underwater adhesion strength (388.1 kPa) to porcine skin. In addition, MXene has been employed to obtain high electrical conductivity, create a route for stable electron transport, and reinforce mechanical properties. The hydrogel also possesses self-healing ability, a low swelling ratio (â¼3.8%), biocompatibility, and specific adhesion to biological tissues in water. Facilitated with these advantages, the hydrogel-based electrodes achieve reliable electrophysiological signal detection in both air and wet conditions and demonstrate a higher signal-to-noise ratio (28.3 dB) than that of commercial Ag/AgCl gel electrodes (18.5 dB). Also, the hydrogel can be utilized as a strain sensor with high sensitivity for underwater communication. This multifunctional hydrogel improves the stability of the skin-hydrogel interface in aquatic environments and is expected to be promising for the next-generation bio-integrated electronics.
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Comunicação , Hidrogéis , Humanos , Suínos , Animais , Edema , Condutividade Elétrica , AdesivosRESUMO
The sturdy chelation of 1,2-diamines and transition-metals would retard or even interrupt the routine catalytic cycles. In the amidation and asymmetric reductive amination (ARA) cascade reactions of diamines and ketoesters, we deployed sets of additives to ensure a smooth transformation catalyzed by the complexes of rhodium and versatile and highly modular phosphoramidite-phosphine ligands. The tunability of the ligands was fully exploited to accommodate various diamines and α-ketoesters for the efficient synthesis of chiral 3,4-dihydroquinoxalinones.