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Wetting and evaporation behavior of dilute sodium dodecyl sulfate (SDS) droplets on planar polydimethylsiloxane (PDMS) surfaces under a direct current (DC) electric field were experimentally investigated. Two characteristic voltages-actuation voltage and saturation voltage were observed in the electrowetting of dilute SDS droplets on PDMS surfaces. It was found that for dilute SDS droplets with a fixed SDS concentration substrate elasticity has an obvious influence on actuation voltage, and saturation voltage increased with the increase of mass ratio of PDMS surfaces. SDS concentration was also found to obviously influence actuation voltage and saturation voltage when SDS concentration was in a certain range. For the case of evaporation of sessile dilute SDS droplets on PDMS surfaces with the application of a DC electric field, substrate elasticity, SDS concentration and the magnitude of applied voltage were all found to have an influence on the duration of CCR stage. Moreover, contact angle hysteresis for dilute SDS droplets on a planar PDMS 10:1 surface under different applied voltage was measured and it was found that the magnitude of applied voltage greatly influenced contact angle hysteresis, which also depends on SDS concentration and KCl concentration.
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Transition metal selenides (TMSs) are viewed as a prospective high-capacity electrode material for asymmetric supercapacitors (ASCs). However, the inability to expose sufficient active sites due to the limitation of the area involved in the electrochemical reaction severely limits their inherent supercapacitive properties. Herein, a self-sacrificing template strategy is developed to prepare self-supported CuCoSe (CuCoSe@rGO-NF) nanosheet arrays by in situ construction of copper-cobalt bimetallic organic framework (CuCo-MOF) on rGO-modified nickel foam (rGO-NF) and rational design of Se2- exchange process. Nanosheet arrays with high specific surface area are considered to be ideal platforms for accelerating electrolyte penetration and exposing rich electrochemical active sites. As a result, the CuCoSe@rGO-NF electrode delivers a high specific capacitance of 1521.6 F/g at 1 A/g, good rate performance and an excellent capacitance retention of 99.5% after 6000 cycles. The assembled ASC device has a high energy density of 19.8 Wh kg-1 at 750 W kg-1 and an ideal capacitance retention of 86.2% after 6000 cycles. This proposed strategy offers a viable strategy for designing and constructing electrode materials with superior energy storage performance.
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The development of flexible microelectronic systems requires the construction of high-energy-output planar micro-supercapacitors (MSCs). Herein, the localized electron density, by introducing graphene quantum dots (GQDs) on the surface of electrodes, is regulated. The enhanced local field intensity promotes ion electrostatic adsorption at the solid-liquid interface, which significantly improves the energy density of MSCs in the confined space. Local electronic structure has been investigated from the perspective of the topological analysis of the electron localization function (ELF) and the electron density. Impressively, the edges of the simulated structure exhibit a higher electron density distribution than the CC skeleton. This finding indicates that the introduced GQDs reinforce the intrinsic electrical double-layer capacitance (EDLC) and the oxygen-bearing functional groups at the edge, further increasing the pseudocapacitance performance. Moreover, the edge electron aggregation effect enables the all-carbon-based symmetric MSCs to exhibit ultra-high areal capacitance (21.78 mF cm-2 ) and excellent cycle stability (86.74% retention after 25 000 cycles). This novel surface local charge regulation strategy is also applied for intensifying ion electrostatic adsorption on Zn-ion hybrid MSCs (polyvalent metal ions) and ion-gel electrolyte MSCs (non-metallic ions). With excellent planar integration, this device demonstrates excellent flexibility and has potential applications in timing and environmental monitoring.
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Electroreduction of nitrate to ammonia, instead of N2, is beneficial toward pollution control and value-added chemical production. Metallic catalysts have been developed for enhancing ammonia evolution efficiency from nitrate based on the crystalline state of the catalyst. However, the development of amorphous metallic catalysts with more active sites is still unexplored. Herein, a highly distributed amorphous Cu catalyst exhibiting an outstanding ammonia yield rate of 1.42 mol h-1 g-1 and Faradaic efficiency of 95.7%, much superior to crystallized Cu, is demonstrated for nitrate-reduction to ammonia. Experimental and computational results reveal that amorphizing Cu increases the number of catalytic sites, enhances the NO3- adsorption strength with flat adsorption configurations, and facilitates the potential determining step of *NO protonation to *NHO. The amorphous Cu catalyst shows good electrochemical stability at - 0.3 V, while crystallization weakens the activity at a more negative potential. This study confirms the crystallinity-activity relationship of amorphous catalysts and unveils their potential-limited electrochemical stability.
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Morphologies of evaporative deposition, which has been widely applied in potential fields, were induced by the competition between internal flows inside evaporating droplets. Controlling the pattern of deposition and suppressing the coffee-ring effect are essential issues of intense interest in the aspects of industrial technologies and scientific applications. Here, evaporative deposition of surfactant-laden nanofluid droplets over silicon was experimentally investigated. A ring-like deposition was formed after complete evaporation of sodium dodecyl sulfate (SDS)-laden nanofluid droplets with an initial SDS concentration ranging from 0 to 1.5 CMC. In the case of initial SDS concentrations above 1.3 CMC, no cracks were observed in the ring-like deposition, indicating that the deposition patterns of nanofluid droplets could be completely changed and cracks could be eliminated by sufficient addition of SDS. With the increase of the initial concentration of hexadecyl trimethylammonium bromide (CTAB), the width of the deposition ring gradually decreased until no ring-like structure was formed. On the contrary, with the increase of the initial Triton X-100 (TX-100) concentration, the width of the deposition ring gradually increased until a uniform deposition was generated. Moreover, when the initial TX-100 concentration was high, a "tree-ring-like" pattern was discovered. Besides, morphologies of evaporative pattern due to the addition of surfacants were qualitatively analyzed.
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Silicon (Si) is attracted much attention due to its outstanding theoretical capacity (4200 mAh/g) as the anode of lithium-ion batteries (LIBs). However, the large volume change and low electron/ion conductivity during the charge and discharge process limit the electrochemical performance of Si-based anodes. Here we demonstrate a foldable acrylic yarn-based composite carbon nanofiber embedded by Si@SiOx particles (Si@SiOx-CACNFs) as the anode material. Since the amorphous SiOx and carbon (C) coating on the outside of the Si particles can provide a double buffer for volume expansion while reducing the contact between the Si core and the electrolyte to form a thin and stable solid electrolyte interface (SEI) film. Simultaneous in-situ electrochemical impedance spectroscopy (in-situ EIS) and galvanostatic intermittent titration technique (GITT) tests show that SiOx and C have higher ion/electron transport rates, and in addition, using acrylic fiber yarn and Zn(Ac)2 as raw materials reduces the manufacturing cost and enhanced mechanical properties. Therefore, the half-cell can achieve a high initial Coulombic efficiency (ICE) of 82.3% and a reversible capacity of 1358.2 mAh/g after 180 cycles. It can return to its original shape and remain intact after four consecutive folds, and the soft-pack full battery can also light up LED lights under different bending conditions.
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Although lithium-sulfur (Li-S) batteries with a high theoretical energy density and low cost have attracted extensive research attention, their commercialization is still unsuccessful due to the poor cycle life caused by the dissolution of polysulfides. It is the key challenge to overcome polysulfide shuttling for achieving long-term cycling stability in Li-S batteries. Here we report a novel strategy for the synthesis of N, S-doped graphene with high nitrogen and sulfur contents via in situ self-assembly of graphene oxide and thiourea-formaldehyde resin and calcination. The N, S-doped graphene serves as a conductive agent and a chemosorbent for suppressing polysulfide shuttling and preventing the Li-metal from corrosion, leading to a high reversible capacity and superior cycling stability. The Li-S batteries with the N, S-doped graphene can achieve an excellent cycling life (622 mA h g-1 after 500 cycles at 1C) and a slow capacity decay rate (0.049% per cycle over 500 cycles at 1C). The proposed strategy has the potential to enhance the high electrochemical properties of Li-S batteries.
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Droplet impact on pillar-arrayed polydimethylsiloxane (PDMS) surfaces with different solid fractions was studied. The lower and upper limits of Weber number, We, for complete rebound of impacting droplets decreased with decreasing solid fractions. Gaps were visible during the spreading and retraction processes of bouncing droplets on the surface with a solid fraction of 0.06 while no gaps were observed during the retraction process when We was greater than its upper limit, indicating that there existed a transition from the Cassie-Baxter wetting state to the Wenzel wetting state. Therefore, a novel model accounting for the penetration of a liquid into the cavities between the pillars was developed to predict the upper limit of the impact velocity of bouncing droplets. At high We, partial rebound was observed for surfaces with solid fractions of 0.50 and 0.20 while a sticky state was observed for the surface with a solid fraction of 0.06. Moreover, surface roughness has a great influence on the contact time of bouncing droplets. Besides, the maximum spreading parameter was found to follow a scaling law of We1/4.
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Evaporation of water and ethanol/water droplets containing large polystyrene (PS) microparticles on polydimethylsiloxane (PDMS) surface was experimentally investigated. It is found that no matter with or without small addition of ethanol, a compact monolayer deposition is formed for lower microparticle concentration while mountain-like deposition for higher concentration. Since the more volatile compound (ethanol) evaporates more quickly than the less volatile compound (water), evaporation of ethanol/water mixture droplet exhibits different characteristics from pure water. When the concentration of microparticle is low, the contact radius of ethanol/water mixture droplet decreases throughout the whole process, while the contact angle increases at first to a maximum, then keeps almost constant, and finally decreases sharply. However, the evaporation of ethanol/water mixture droplet with higher concentration of microparticle behaviors more complex. The settling time of microparticles was estimated and its theoretical value agrees well with the experimental one. Moreover, a mechanism of self-pinning of microparticles was used to elucidate the deposition behavior of microparticles, indicating that as the contact line is depinning, the liquid film covering the outmost microparticle becomes thicker and thicker, and the microparticles have to move spontaneously with the depinning contact line under the action of capillary force.
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Experiments of sessile water droplet evaporation on both polydimethylsiloxane (PDMS) and Teflon surfaces were conducted. All experiments begin with constant contact area mode (the initial contact angle is greater than 90°), switch to constant contact angle mode and end with mixed mode. Based on the assumptions of spherical droplet and uniform concentration gradient, theoretical analyses for both constant contact area and constant contact angle modes are made and theoretical solutions are derived accordingly, especially a theoretical solution of contact angle is presented first for CCR stage with any value of the initial contact angle. Moreover, comparisons between the theoretical solutions and experimental data of contact angle in CCR stage demonstrate the validity of the theoretical solution and it would help for a better understanding and application of water droplet on solid surfaces, which is quite often encountered in lab-on-a-chip, polymerase chain reaction (PCR) and other micro-fluidics devices.
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In this paper, the role of vertical component of surface tension of a droplet on the elastic deformation of a finite-thickness flexible membrane was theoretically analyzed using Hankel transformation. The vertical displacement at the surface was derived and can be reduced to Lester's or Rusanov's solutions when the thickness is infinite. Moreover, some simulations of the effect of a liquid droplet on a membrane with a finite thickness were made. The numerical results showed that there exists a saturated membrane thickness of the order of millimeter, when the thickness of a membrane is larger than such a value, the membrane can be regarded as a half-infinite body. Further numerical calculations for soft membrane whose thickness is far below the saturated thickness were made. By comparison between the maximum vertical displacement of an ultrathin soft membrane and a half-infinite body, we found that Lester's or Rusanov's solutions for a half-infinite body cannot correctly describe such cases. In other words, the thickness of a soft membrane has great effect on the surface deformation of the ultrathin membrane induced by a liquid droplet.
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In this paper, we studied the role of vertical component of surface tension of a water droplet on the deformation of membranes and microcantilevers (MCLs) widely used in lab-on-a-chip and micro- and nano-electromechanical system (MEMS/NEMS). Firstly, a membrane made of a rubber-like material, poly(dimethylsiloxane) (PDMS), was considered. The deformation was investigated using the Mooney-Rivlin (MR) model and the linear elastic constitutive relation, respectively. By comparison between the numerical solutions with two different models, we found that the simple linear elastic model is accurate enough to describe such kind of problem, which would be quite convenient for engineering applications. Furthermore, based on small-deflection beam theory, the effect of a liquid droplet on the deflection of a MCL was also studied. The free-end deflection of the MCL was investigated by considering different cases like a cylindrical droplet, a spherical droplet centered on the MCL and a spherical droplet arbitrarily positioned on the MCL. Numerical simulations demonstrated that the deflection might not be neglected, and showed good agreement with our theoretical analyses.