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Crumlin, Ethan J. "(Invited) Using Ambient Pressure XPS to Probe the Solid/Gas and Solid/Liquid Interface Under in Situ and Operando Conditions." ECS Meeting Abstracts MA2022-02, no. 46 (October 9, 2022): 1715. http://dx.doi.org/10.1149/ma2022-02461715mtgabs.
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Interfaces play an essential role in nearly all aspects of life and are critical for electrochemistry. Prof. Robert Savinell has played a pivotal interface to me in the role of mentorship in both life and electrochemistry, and I look to honor his contributions to both through this talk. Electrochemical systems ranging from high-temperature solid oxide fuel cells (SOFC) to batteries to capacitors have a wide range of important interfaces between solids, liquids, and gases, which play a pivotal role in how energy is stored, transferred, and converted. I will share the use of ambient pressure XPS (APXPS) to directly probe the solid/gas and solid/liquid electrochemical interface. APXPS is a photon-in/electron-out process that can provide both atomic concentration and chemical-specific information at pressures greater than 20 Torr. Using synchrotron X-rays at Lawrence Berkeley Nation Laboratory, the Advanced Light Source has several beamlines dedicated to APXPS endstations that are outfitted with various in situ/operando features such as heating to temperatures > 500 °C, pressures greater than 20 Torr to support solid/liquid experiments and electrical leads to support applying electrical potentials support the ability to collect XPS data of actual electrochemical devices while it's operating in near ambient pressures. This talk will introduce APXPS and provide several interface electrochemistry examples using in situ and operando APXPS, including the probing of Sr segregation on a SOFC electrode to a Pt metal electrode undergoing a water-splitting reaction to generate oxygen, the ability to measure the electrochemical double layer (EDL) to our most recent efforts to directly probe an ion exchange membranes Donnan potential. Gaining new insight to guide the design and control of future electrochemical interfaces and how Bob, electrochemistry, and I have interfaced over the years.
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Josell, Daniel, and Frans Spaepen. "Surfaces, Interfaces, and Changing Shapes in Multilayered Films." MRS Bulletin 24, no. 2 (February 1999): 39–43. http://dx.doi.org/10.1557/s0883769400051538.
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It is generally recognized that the capillary forces associated with internal and external interfaces affect both the shapes of liquid-vapor surfaces and wetting of a solid by a liquid. It is less commonly understood that the same phenomenology often applies equally well to solid-solid or solid-vapor interfaces.The fundamental quantity governing capillary phenomena is the excess free energy associated with a unit area of interface. The microscopic origin of this excess free energy is often intuitively simple to understand: the atoms at a free surface have “missing bonds”; a grain boundary contains “holes” and hence does not have the optimal electronic density; an incoherent interface contains dislocations that cost strain energy; and the ordering of a liquid near a solid-liquid interface causes a lowering of the entropy and hence an increase in the free energy. In what follows we shall show how this fundamental quantity determines the shape of increasingly complex bodies: spheres, wires, thin films, and multilayers composed of liquids or solids. Crystal anisotropy is not considered here; all interfaces and surfaces are assumed isotropic.Consideration of the equilibrium of a spherical drop of radius R with surface free energy γ shows that pressure inside the droplet is higher than outside. The difference is given by the well-known Laplace equation:This result can be obtained by equating work done against internal and external pressure during an infinitesimal change of radius with the work of creating a new surface.
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Saleman, Abdul Rafeq, Mohamad Shukri Zakaria, Ridhwan Jumaidin, Nur Hazwani Mokhtar, and Nor Aslily Sarkam. "Molecular Dynamics Study: Correlation of Heat Conduction Across S-L Interfaces Between Constant Heat Flux and Shear Applied to Liquid Systems." Journal of Mechanical Engineering 19, no. 3 (September 15, 2022): 33–53. http://dx.doi.org/10.24191/jmeche.v19i3.19795.
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Heat conduction (HC) at solid-liquid (S-L) interfaces play a significant role in the performance of engineering systems. Thus, this study investigates HC at S-L interfaces and its correlation between constant heat flux (CHF) and shear applied to liquid (SAL) systems using non-equilibrium molecular dynamics simulation. The S-L interface consists of solids with the face-centred cubic (FCC) lattice of (110), (111) and (100) planes facing the liquid. The solid is modelled by Morse potential whereas the liquid is modelled by Lennard Jones potential. The interaction between solid-liquid was modelled by Lorentz-Bertholet combining rules. The temperature and heat flux of the system is evaluated to correlate the HC at the S-L interface which reflect by the interfacial thermal resistance (ITR). The results suggest that the surfaces of FCC influence ITR at the S-L interface. The (110) surface for both cases of CHF and SAL has the lowest ITR as compared to other surfaces. In general, ITR for the case of SAL is higher than the CHF. SAL disturbs the adsorption behaviour of liquid at the S-L interfaces, thus reducing the HC. In conclusion, the surface of FCC and liquid experiencing shear do influence the characteristics of HC at the S-L interface.
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Streubel, Robert, Xubo Liu, Xuefei Wu, and Thomas P. Russell. "Perspective: Ferromagnetic Liquids." Materials 13, no. 12 (June 15, 2020): 2712. http://dx.doi.org/10.3390/ma13122712.
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Mechanical jamming of nanoparticles at liquid–liquid interfaces has evolved into a versatile approach to structure liquids with solid-state properties. Ferromagnetic liquids obtain their physical and magnetic properties, including a remanent magnetization that distinguishes them from ferrofluids, from the jamming of magnetic nanoparticles assembled at the interface between two distinct liquids to minimize surface tension. This perspective provides an overview of recent progress and discusses future directions, challenges and potential applications of jamming magnetic nanoparticles with regard to 3D nano-magnetism. We address the formation and characterization of curved magnetic geometries, and spin frustration between dipole-coupled nanostructures, and advance our understanding of particle jamming at liquid–liquid interfaces.
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Veen, J. F. van der, and H. Reichert. "Structural Ordering at the Solid–Liquid Interface." MRS Bulletin 29, no. 12 (December 2004): 958–62. http://dx.doi.org/10.1557/mrs2004.267.
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AbstractMany processes in nature and technology are based on the static and dynamic properties of solid–liquid interfaces. Prominent examples are crystal growth, melting, and recrystallization. These processes are strongly affected by the local structure at the solid–liquid interface. Therefore, it is mandatory to understand the change in the structure across the interface. The break of the translational symmetry at the interface induces ordering phenomena, and interactions between the liquid's molecules and the atomically corrugated solid surface may induce additional ordering effects. In the past decade, new techniques have been developed to investigate the structural properties of such (deeply) buried interfaces in their natural environment. These methods are based on deeply penetrating probes such as brilliant x-ray beams, providing full access to the structure parallel and perpendicular to the interface. Here, we review the results of a number of case studies including liquid metals in contact with Group IV elements (diamond and silicon), where charge transfer effects at the interface may come into play. Another particularly important liquid in our environment is water. The structural properties of water vary widely as it is brought in contact with other materials. We will then proceed from these seemingly simple cases to complex fluids such as colloids.
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Titova, E. A., and D. V. Alexandrov. "The boundary integral equation for curved solid/liquid interfaces propagating into a binary liquid with convection." Journal of Physics A: Mathematical and Theoretical 55, no. 5 (January 11, 2022): 055701. http://dx.doi.org/10.1088/1751-8121/ac463e.
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Abstract The boundary integral method is developed for unsteady solid/liquid interfaces propagating into undercooled binary liquids with convection. A single integrodifferential equation for the interface function is derived using the Green function technique. In the limiting cases, the obtained unsteady convective boundary integral equation transforms into a previously developed theory. This integral is simplified for the steady-state growth in arbitrary curvilinear coordinates when the solid/liquid interface is isothermal (isoconcentration). Finally, we evaluate the boundary integral for a binary melt with a forced flow and analyze how the melt undercooling depends on Péclet and Reynolds numbers.
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Briant, C. L. "Grain Boundary Chemistry and Reactions in Metals." MRS Bulletin 15, no. 10 (October 1990): 26–32. http://dx.doi.org/10.1557/s0883769400058632.
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An interface can be defined as a surface that serves as a common boundary between two phases. Examples include the boundaries between two solids, two immiscible liquids, a solid and a liquid, a solid and a gas, and a liquid and a gas. Interfaces have been studied for decades by scientists of many different disciplines. One reason for this interest is that the atomic structure and the chemical composition at the interface can differ from that of the bulk material on either side of it. Consequently, the properties of the interface can differ greatly from those of either bulk phase, and chemical reactions can occur more readily at the interface than in the bulk.All the interfaces listed in the previous paragraph are of interest to materials scientists. However, this article will only consider the grain boundary because it has received the most attention by researchers in materials science. Furthermore, we will only consider grain boundaries in metals; nonmetallic systems will be covered in other articles in this issue.A grain boundary is an interface that exists where two single crystals are joined in such a way that their crystallographic orientations are not completely matched. Thus, any polycrystalline material contains many grain boundaries. They occur wherever the individual grains meet one another and can usually be observed by etching a polished cross section of the surface as shown in Figure 1. Grain boundaries first form in a metal as a result of the multiple nucleation sites that occur during solidification.
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Giunta, Giuliana, and Paola Carbone. "Cross-over in the dynamics of polymer confined between two liquids of different viscosity." Interface Focus 9, no. 3 (April 19, 2019): 20180074. http://dx.doi.org/10.1098/rsfs.2018.0074.
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Using molecular dynamics simulations, we analysed the polymer dynamics of chains of different molecular weights entrapped at the interface between two immiscible liquids. We showed that on increasing the viscosity of one of the two liquids the dynamic behaviour of the chain changes from a Zimm-like dynamics typical of dilute polymer solutions to a Rouse-like dynamics where hydrodynamic interactions are screened. We observed that when the polymer is in contact with a high viscosity liquid, the number of solvent molecules close to the polymer beads is reduced and ascribed the screening effect to this reduced number of polymer–solvent contacts. For the longest chain simulated, we calculated the distribution of loop length and compared the results with the theoretical distribution developed for solid/liquid interfaces. We showed that the polymer tends to form loops (although flat against the interface) and that the theory works reasonably well also for liquid/liquid interfaces.
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Howe, J. M. "Quantification of order in the liquid at a solid-liquid interface by high-resolution transmission electron microscopy (HRTEM)." Proceedings, annual meeting, Electron Microscopy Society of America 54 (August 11, 1996): 114–15. http://dx.doi.org/10.1017/s0424820100163034.
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A number of different theoretical approaches have been used to model the atomic structure and properties of solid-liquid interfaces. Most calculations indicate that ordering occurs in the first several layers of the liquid, adjacent to the crystal surface. In contrast to the numerous theoretical investigations, there have been no direct experimental observations of the atomic structure of a solid-liquid interface for comparison. Saka et al. examined solid-liquid interfaces in In and In-Sb at lattice-fringe resolution in the TEM, but their data do not reveal information about the atomic structure of the liquid phase. The purpose of this study is to determine the atomic structure of a solid-liquid interface using a highly viscous supercooled liquid, i.e., a crystal-amorphous interface.
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Pascall, Andrew J., and Todd M. Squires. "Electrokinetics at liquid/liquid interfaces." Journal of Fluid Mechanics 684 (September 28, 2011): 163–91. http://dx.doi.org/10.1017/jfm.2011.288.
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AbstractElectrokinetic effects at liquid/liquid interfaces have received considerably less attention than at solid/liquid interfaces. Because liquid/liquid interfaces are generally mobile, one might expect electrokinetic effects over a liquid/liquid interface to be faster than over an equivalent solid surface. The earliest predictions for the electrophoretic mobility of charged mercury drops – distinct approaches by Frumkin, along with Levich, and Booth – differed by $O(a/ {\lambda }_{D} )$, where $a$ is the radius of the drop and ${\lambda }_{D} $ is the Debye length. Seeking to reconcile this rather striking discrepancy, Levine & O’Brien showed double-layer polarization to be the key ingredient. Without a physical mechanism by which electrokinetic effects are enhanced, however, it is difficult to know how general the enhancement is – whether it holds only for liquid metal surfaces, or more generally, for all liquid/liquid surfaces. By considering a series of systems in which a planar metal strip is coated with either a liquid metal or liquid dielectric, we show that the central physical mechanism behind the enhancement predicted by Frumkin is the presence of an unmatched electrical stress upon the electrolyte/liquid interface, which establishes a Marangoni stress on the droplet surface and drives it into motion. The source of the unbalanced electrokinetic stress on a liquid metal surface is clear – metals represent equipotential surfaces, so no field exists to drive an equal and opposite force on the surface charge. This might suggest that liquid metals represent a unique system, since dielectric liquids can support finite electric fields, which might be expected to exert an electrical stress on the surface charge that balances the electric stress. We demonstrate, however, that electrical and osmotic stresses on relaxed double layers internal to dielectric liquids precisely cancel, so that internal electrokinetic stresses generally vanish in closed, ideally polarizable liquids. The enhancement predicted by Frumkin for liquid mercury drops can thus be expected quite generally over ideally polarizable liquid drops. We then reconsider the electrophoretic mobility of spherical drops, and reconcile the approaches of Frumkin and Booth: Booth’s neglect of double-layer polarization leads to a standard electro-osmotic flow, without the enhancement, and Frumkin’s neglect of the detailed double-layer dynamics leads to the enhanced electrocapillary motion, but does not capture the (sub-dominant) electrophoretic motion. Finally, we show that, while the electrokinetic flow over electrodes coated with thin liquid films is $O(d/ {\lambda }_{D} )$ faster than over solid/liquid interfaces, the Dukhin number, $\mathit{Du}$, which reflects the importance of surface conduction to bulk conduction, generally increases by a smaller amount [$O(d/ L)$], where $d$ is the thickness of film and $L$ is the length of the electrode. This suggests that liquid/liquid interfaces may be utilized to enhance electrokinetic velocities in microfluidic devices, while delaying the onset of high-$\mathit{Du}$ electrokinetic suppression.
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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
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Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.
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Spencer Jolly, Dominic, Dominic L. R. Melvin, Isabella D. R. Stephens, Rowena H. Brugge, Shengda D. Pu, Junfu Bu, Ziyang Ning, et al. "Interfaces between Ceramic and Polymer Electrolytes: A Comparison of Oxide and Sulfide Solid Electrolytes for Hybrid Solid-State Batteries." Inorganics 10, no. 5 (April 26, 2022): 60. http://dx.doi.org/10.3390/inorganics10050060.
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Hybrid solid-state batteries using a bilayer of ceramic and solid polymer electrolytes may offer advantages over using a single type of solid electrolyte alone. However, the impedance to Li+ transport across interfaces between different electrolytes can be high. It is important to determine the resistance to Li+ transport across these heteroionic interfaces, as well as to understand the underlying causes of these resistances; in particular, whether chemical interphase formation contributes to giving high resistances, as in the case of ceramic/liquid electrolyte interfaces. In this work, two ceramic electrolytes, Li3PS4 (LPS) and Li6.5La3Zr1.5Ta0.5O12 (LLZTO), were interfaced with the solid polymer electrolyte PEO10:LiTFSI and the interfacial resistances were determined by impedance spectroscopy. The LLZTO/polymer interfacial resistance was found to be prohibitively high but, in contrast, a low resistance was observed at the LPS/polymer interface that became negligible at a moderately elevated temperature of 50 °C. Chemical characterization of the two interfaces was carried out, using depth-profiled X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry, to determine whether the interfacial resistance was correlated with the formation of an interphase. Interestingly, no interphase was observed at the higher resistance LLZTO/polymer interface, whereas LPS was observed to react with the polymer electrolyte to form an interphase.
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Storaska, Garrett A., and James M. Howe. "In-Situ TEM Investigation of the Solid/Liquid Interface in Al-Si Alloys." Microscopy and Microanalysis 6, S2 (August 2000): 1068–69. http://dx.doi.org/10.1017/s1431927600037831.
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The solid/liquid interface is a junction between two condensed phases with completely different atomic arrangements. At the interface between the periodically ordered solid and the amorphous liquid, the atoms adopt a structure that minimizes the excess energy due to the abrupt change between the surrounding phases. Faceted and diffuse interfaces describe two extremes in morphology of a solid/liquid interface. In a faceted interface, the change from solid to liquid occurs over one atomic layer, however periodic order extends into the first few liquid layers adjacent to the crystalline solid, as predicted by numerous models.1 The faceted interface advances by nucleation and growth of ledges on the interface. A diffuse interface has a structure in which the change from solid to liquid occurs over several atomic layers. This interface contains many ledges to which liquid atoms may attach continuously as the interface advances.
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Saka, H., K. Sasaki, S. Tsukimoto, and S. Arai. "In situ Observation of Solid–liquid Interfaces by Transmission Electron Microscopy." Journal of Materials Research 20, no. 7 (July 1, 2005): 1629–40. http://dx.doi.org/10.1557/jmr.2005.0212.
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Recent progress in in situ observation of solid–liquid interfaces by means of transmission electron microscopy, carried out by the Nagoya group, was reviewed. The results obtained on pure materials are discussed based on Jackson's theory. The structure of the solid–liquid interfaces of eutectic alloys was also observed. The in situ observation technique of solid–liquid interface is applied to industrially important reactions which include liquid phases.
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Kurihara, Kazue. "Surface forces measurement for materials science." Pure and Applied Chemistry 91, no. 4 (April 24, 2019): 707–16. http://dx.doi.org/10.1515/pac-2019-0101.
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Abstract This article reviews the surface forces measurement as a novel tool for materials science. The history of the measurement is briefly described in the Introduction. The general overview covers specific features of the surface forces measurement as a tool for studying the solid-liquid interface, confined liquids and soft matter. This measurement is a powerful way for understanding interaction forces, and for characterizing (sometime unknown) phenomena at solid-liquid interfaces and soft complex matters. The surface force apparatus (SFA) we developed for opaque samples can study not only opaque samples in various media, but also electrochemical processes under various electrochemical conditions. Electrochemical SFA enables us to determine the distribution of counterions between strongly bound ones in the Stern layer and those diffused in the Gouy-Chapman layer. The shear measurement is another active area of the SFA research. We introduced a resonance method, i.e. the resonance shear measurement (RSM), that is used to study the effective viscosity and lubricity of confined liquids in their thickness from μm to contact. Advantages of these measurements are discussed by describing examples of each measurement. These studies demonstrate how the forces measurement is used for characterizing solid-liquid interfaces, confined liquids and reveal unknown phenomena. The readers will be introduced to the broad applications of the forces measurement in the materials science field.
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You, Hoydoo, and Zoltán Nagy. "Applications of Synchrotron Surface X-Ray Scattering Studies of Electrochemical Interfaces." MRS Bulletin 24, no. 1 (January 1999): 36–40. http://dx.doi.org/10.1557/s088376940005171x.
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Aqueous-solution/solid interfaces are ubiquitous in modern manufacturing environments as well as in our living environment, and studies of such interfaces are an active area of science and engineering research. An important area is the study of liquid/solid interfaces under active electrochemical control, which has many immediate technological implications, for example, corrosion/passivation of metals and energy storage in batteries and ultracapacitors. The central phenomenon of electrochemistry is the charge transfer at the interface, and the region of interest is usually wider than a single atomic layer, ranging from a monolayer to thousands of angstroms, extending into both phases.Despite the technological and environmental importance of liquid/solid interfaces, the atomic level understanding of such interfaces had been very much hampered by the absence of nondestructive, in situ experimental techniques. The situation has changed somewhat in recent decades with the development of the largely ex situ ultrahigh vacuum (UHV) surface science, modern spectroscopic techniques, and modern surface microscopy.However in situ experiments of electrochemical interfaces are difficult, stemming from the special nature of these interfaces. These are so-called buried interfaces in which the solid electrode surface is covered by a relatively thick liquid layer. For this reason, the probe we use in the structural investigation must satisfy simultaneously two conditions: (1) the technique must be surface/interface sensitive, and (2) absorption of the probe in the liquid phase must be sufficiently small for penetration to and from the interface of interest without significant intensity loss.
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Alexandrova, Lidia A., Ljudmil S. Grigorov, Nikolay A. Grozev, and Stoyan I. Karakashev. "Investigation of Interfacial Free Energy of Three-Phase Contact on a Glass Sphere in Case of Cationic-Anionic Surfactant Aqueous Mixtures." Coatings 10, no. 6 (June 18, 2020): 573. http://dx.doi.org/10.3390/coatings10060573.
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The wetting of adsorbed surfactants solids is important for various technological applications in particular for the process of foam flotation. The present work aims at calculating the surface tensions of the three phase interfaces at different surfactant concentrations using the Girifalco and Good method. For this purpose, the surface tension and contact angle vs. surfactant concentration of the test substances amines and sulfonates and their mixture were measured for liquid–air interface. Calculated surface tension of solid–air interface vs. concentration for C10 amine and mixed systems are close to those for the liquid–air surface, but are slightly lower. In the case of mixed systems, the graph has a specific structure similar to that of liquid–air surface dependence. In contrast to the solid–air interface results, the solid–liquid surface tension values are significantly lower. In case of the mixed surfactant systems, C10amine/C10 sulfonate, a synergetic effect on the surface tension is observed. The specific behavior of the mixed systems is interpreted with the emergence of aggregates consisting of the anionic and cationic surfactants. It is shown that in the whole area of concentrations complete wetting does not occur.
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Fan, Feng Ru. "(Invited) novel Charged Interfaces for Catalysis and Energy Conversion." ECS Meeting Abstracts MA2023-01, no. 34 (August 28, 2023): 1885. http://dx.doi.org/10.1149/ma2023-01341885mtgabs.
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Charged interfaces are ubiquitous in many research fields such as electrochemistry, catalysis, and energy chemistry, and are key places where physical and chemical processes occur. The charged interface structure can also be affected by external fields such as light, electricity, and force, and becomes the key to regulating chemical reactions. It is of great significance for the development of surface and interface science, electrochemistry, catalysis and energy science to deeply understand the physical and chemical reaction process and mechanism of various charged interface systems, and to clarify the interaction between interface structure and reacting species. It is extremely challenging to rationally design, construct, and characterize various novel charged interfaces, and then comprehensively and deeply study their physical and chemical processes and mechanisms. By constructing new charged interface structures such as solid/solid triboelectric interface, micro-droplet charged liquid/gas interface, and metal/two-dimensional material charged interface, we study the reaction process and mechanism of the charged interface and develop new energy conversion pathways. A series of innovative research results: Discovered a new mechanism of triboelectric power generation, expanding the new direction of charged interface structure in energy conversion; established and developed epitaxial growth modes of various interface structures; accurately characterized the electron transport of charged interface structure and surface charge distribution and other physical and chemical properties. We have developed new systems such as solid/dielectric/liquid charged interfaces based on electrodes/dielectric layers/electrolytes and liquid/gas charged interfaces based on microdroplets, and explored new applications in energy conversion and electrocatalysis. Applying a voltage to the electrode/dielectric layer/electrolyte interface can polarize the dielectric layer and adsorb ions in the electrolyte, forming a special "sandwich" electric double layer. Different from the solid/solid charged interface formed by triboelectrification or light excitation, this is a new solid/dielectric/liquid charged interface system based on electrostatic adsorption. Based on this interface system, a new nanoscale power generation device is designed, which can effectively convert mechanical energy into electrical energy, and has high output performance. A new liquid/gas charged interface based on micro-droplets was constructed by means of electrospray, a new strategy for confining the liquid/gas charged interface was proposed, and a high-performance electrolytic water catalyst was prepared. The physical and chemical mechanism of accelerated chemical reactions at the liquid/gas charged interface is revealed, and the desolvation effect and interface confinement effect are proved to be effective ways to construct defect-rich electrocatalysts.
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Howe, James M., and Hiroyasu Saka. "In Situ Transmission Electron Microscopy Studies of the Solid–Liquid Interface." MRS Bulletin 29, no. 12 (December 2004): 951–57. http://dx.doi.org/10.1557/mrs2004.266.
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AbstractIn situtransmission electron microscopy (TEM) studies allow one to determine the structure, chemistry, and kinetic behavior of solid–liquid (S–L) interfaces with subnanometer spatial resolution. This article illustrates some important contributions ofin situTEM to our understanding of S–L interfaces in Al-Si alloys and liquid In particles in Al and Fe matrices.Four main areas are discussed:ordering in the liquid at a S–L interface, compositional changes across the interface, the kinetics and mechanisms of interface migration, and the contact angles and equilibrium melting temperature of small particles.Results from these studies reveal that (1)partially ordered layers form in the liquid at a Si{111} S–L interface in an Al–Si alloy, (2)the crystalline and compositional changes occur simultaneously across an Al S–L interface, (3)the Al interface is diffuse and its growth can be followed at velocities of a fewnm/s at extremely low undercoolings, and (4)the melting temperature of In particles less than ~ 10 nm in diameter can be raised or lowered in Al or Fe, depending on the contact angle that the S–L interface makes at the three-phase junction. These results illustrate the benefits of in situ TEM for providing fundamental insight into the mechanisms that control the behavior of S–L interfaces in materials.
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Spaepen, Frans. "Structure of Liquids and Solid-Liquid Interfaces." Bulletin de la Classe des sciences 14, no. 1 (2003): 195–96. http://dx.doi.org/10.3406/barb.2003.28361.
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Paris, Oskar, Barbara Aichmayer, and Peter Fratzl. "Small-angle scattering from spherical particles on randomly oriented interfaces." International Journal of Materials Research 97, no. 3 (March 1, 2006): 290–94. http://dx.doi.org/10.1515/ijmr-2006-0046.
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Abstract Small-angle scattering (SAS) has long been used to study nucleation and growth of particles in solid or liquid matrices. In some special cases, nucleation of particles occurs on interfaces, e. g., grain boundaries in crystalline solids or membranes in a solvent. Clearly, the position of the particles is constrained in this case to a narrow region close to the interface, which leads to correlations between the particles. In the present paper, we derive simple expressions for the analysis of SAS data from particles located on planar interfaces, and compare the analytical approximations with computer simulations.
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Negahdar, Leila, Christopher M. A. Parlett, Mark A. Isaacs, Andrew M. Beale, Karen Wilson, and Adam F. Lee. "Shining light on the solid–liquid interface: in situ/operando monitoring of surface catalysis." Catalysis Science & Technology 10, no. 16 (2020): 5362–85. http://dx.doi.org/10.1039/d0cy00555j.
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Many industrially important chemical transformations occur at the interface between a solid catalyst and liquid reactants. In situ and operando spectroscopies offer unique insight into the reactivity of such catalytically active solid–liquid interfaces.
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CHAUDHURI, ABHISHEK, DEBASISH CHAUDHURI, and SURAJIT SENGUPTA. "INDUCED INTERFACES AT NANOSCALES: STRUCTURE AND DYNAMICS." International Journal of Nanoscience 04, no. 05n06 (October 2005): 995–99. http://dx.doi.org/10.1142/s0219581x05003966.
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We show how interfaces may be induced in materials using external fields. The structure and the dynamics of these interfaces may then be manipulated externally to achieve desired properties. We discuss three types of such interfaces: an Ising interface in a nonuniform magnetic field, a solid–liquid interface and an interface between a solid and a smectic like phase. In all of these cases we explicitly show how small size, leading to atomic-scale discreteness and stiff constraints produce interesting effects which may have applications in the fabrication of nanostructured materials.
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Nemoshkalenko, V. V., O. P. Fedorov, E. I. Zhivolub, E. I. Bersudsky, and G. P. Chemerinsky. "«Morphos» Experiment Experimental study of solid-liquid interface in transparent substances." Kosmìčna nauka ì tehnologìâ 6, no. 4 (July 30, 2000): 135–36. http://dx.doi.org/10.15407/knit2000.04.151.
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Zhao, Yu Hong, Wei Jin Liu, Hua Hou, and Yu Hui Zhao. "Impact on Solidification Dendrite Growth by Interfacial Atomic Motion Time with Phase Field Method." Materials Science Forum 749 (March 2013): 660–67. http://dx.doi.org/10.4028/www.scientific.net/msf.749.660.
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The Phase Field model of solidification processes was carried out coupled with temperature field model. The influence of interface atomic time on dendrite growth morphology in undercooled melt was simulated with pure nickel. The experimental results show that when the interface atomic motion time parameter is minor, the liquid-solid interfaces were unstable, disturbance can be amplified easily so the complicated side branches will grow, and the disturbance speed up the dendrite growth. With the increase of , the liquid-solid interfaces become more stable and finally the smooth dendrite morphology can be obtained.
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Chuiko, Myroslava, Lidiia Vytvytska, and Nataliia Pindus. "Method and device for the control of surface properties of porous solids at the boundary of their contact with liquids and gases." Ukrainian Metrological Journal, no. 2 (July 2, 2021): 55–59. http://dx.doi.org/10.24027/2306-7039.2.2021.236089.
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The article indicates the relevance of the problem of controlling the surface properties of solids, analyzes the features of interaction between porous solids in direct contact with liquids.
The process of adhesive interaction of the system “liquid – porous solid” at the interface of these phases is analyzed and the dependence of the degree of wetting by a liquid of the surface of a solid on the structure of the porous body and the surface properties of the liquid is established. The dependence of the contact angle hysteresis of the solid with liquid on the porosity and roughness of the sample of the controlled body is substantiated.
A method of complex express control of the wetting process, which consists in determining the hysteresis of fluid flowing in and out from the surface of a solid body, has been proposed. The method consists in determining the rate of liquid outflow from a tilted sample of a solid. At the same time, the liquid is applied with the same speed to the surface of a porous body sample. The design of device for realization of the method has been developed.
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Lee, Joon-Hyung, Jeong-Joo Kim, Haifeng Wang, and Sang-Hee Cho. "Observation of Intergranular Films in BaB2O4-added BaTiO3 Ceramics." Journal of Materials Research 15, no. 7 (July 2000): 1600–1604. http://dx.doi.org/10.1557/jmr.2000.0229.
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Distribution characteristics of boundary phase in BaB2O4 added BaTiO3 ceramics were investigated with a focus on the curvature difference of solid–liquid interfaces at two-grain and triple junctions. High-resolution transmission electron microscopy revealed that the triple junction of solid grains showed the positive curvature of solid–liquid interface and consisted of the mixture of liquid phase and crystallized BaB2O4 phase. On the other hand, flat amorphous thin film of 2.5-nm thickness was observed at the two-grain junction. This kind of boundary phase distribution characteristic was explained by the solubility difference between two kinds of junctions of solid grains that had different curvature of solid–liquid interfaces.
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Aharon, Hannah, Omer Shavit, Matan Galanty, and Adi Salomon. "Second Harmonic Generation for Moisture Monitoring in Dimethoxyethane at a Gold-Solvent Interface Using Plasmonic Structures." Nanomaterials 9, no. 12 (December 16, 2019): 1788. http://dx.doi.org/10.3390/nano9121788.
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Second harmonic generation (SHG) is forbidden from most bulk metals because metals are characterized by centrosymmetric symmetry. Adsorption or desorption of molecules at the metal interface can break the symmetry and lead to SHG responses. Yet, the response is relatively low, and minute changes occurring at the interface, especially at solid/liquid interfaces, like in battery electrodes are difficult to assess. Herein, we use a plasmonic structure milled in a gold electrode to increase the overall SHG signal from the interface and gain information about small changes occurring at the interface. Using a specific homebuilt cell, we monitor changes at the liquid/electrode interface. Specifically, traces of water in dimethoxyethane (DME) have been detected following changes in the SHG responses from the plasmonic structures. We propose that by plasmonic structures this technique can be used for assessing minute changes occurring at solid/liquid interfaces such as battery electrodes.
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Wang, Xiaoyu, Cynthia J. Jameson, and Sohail Murad. "Interfacial Thermal Conductivity and Its Anisotropy." Processes 8, no. 1 (December 24, 2019): 27. http://dx.doi.org/10.3390/pr8010027.
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There is a significant effort in miniaturizing nanodevices, such as semi-conductors, currently underway. However, a major challenge that is a significant bottleneck is dissipating heat generated in these energy-intensive nanodevices. In addition to being a serious operational concern (high temperatures can interfere with their efficient operation), it is a serious safety concern, as has been documented in recent reports of explosions resulting from many such overheated devices. A significant barrier to heat dissipation is the interfacial films present in these nanodevices. These interfacial films generally are not an issue in macro-devices. The research presented in this paper was an attempt to understand these interfacial resistances at the molecular level, and present possibilities for enhancing the heat dissipation rates in interfaces. We demonstrated that the thermal resistances of these interfaces were strongly anisotropic; i.e., the resistance parallel to the interface was significantly smaller than the resistance perpendicular to the interface. While the latter is well-known—usually referred to as Kapitza resistance—the anisotropy and the parallel component have previously been investigated only for solid-solid interfaces. We used molecular dynamics simulations to investigate the density profiles at the interface as a function of temperature and temperature gradient, to reveal the underlying physics of the anisotropy of thermal conductivity at solid-liquid, liquid-liquid, and solid-solid interfaces.
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Heinze, M. T., J. C. Zill, J. Matysik, W. D. Einicke, R. Gläser, and A. Stark. "Solid–ionic liquid interfaces: pore filling revisited." Phys. Chem. Chem. Phys. 16, no. 44 (2014): 24359–72. http://dx.doi.org/10.1039/c4cp02749c.
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Spencer, B. J., S. H. Davis, G. B. McFadden, and P. W. Voorhees. "Effects of Elastic Stress on the Stability of a Solid-Liquid Interface." Applied Mechanics Reviews 43, no. 5S (May 1, 1990): S54—S55. http://dx.doi.org/10.1115/1.3120850.
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The effects of elastic stress on the stability of solid-liquid interfaces under a variety of conditions are discussed. In the cases discussed, the nonuniform composition field in the solid, which accompanies either the melting process or the development of a perturbation on the solid-liquid interface during solidification, generates nonhydrostatic stresses in the solid. Such compositionally generated elastic stresses have been shown experimentally to induce a solidifying solid-liquid interface to become unstable. We are in the process of analyzing the effects of these stresses on the conditions for morphological stability of a directionally solidified binary alloy.
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Zhuang, Tieshuan, Jun Wu, Tao Zhang, and Xiangwei Dong. "A weakly compressible smoothed particle hydrodynamics framework for melting multiphase flow." AIP Advances 12, no. 2 (February 1, 2022): 025329. http://dx.doi.org/10.1063/5.0057583.
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In this study, the transient process of solid–liquid phase change is modeled and simulated by the multiphase smoothed particle hydrodynamics (SPH) method. First, to simulate the interfacial behaviors of melt liquids, the multiphase SPH model is established for immiscible viscous fluids with a large density ratio, where the environmental liquid surrounding the solid phase is considered, and the surface tension of the melt liquid can be accurately modeled by the continuum surface force method. Based on the multiphase model, the thermal dynamics model is incorporated to describe the heat conduction process. The solid–liquid phase change is realized by directly switching the state of the concerned SPH particle, where the absorbed latent heat is computed by the phase change model. Second, the model is validated by several simulation cases, including the Stefan problem, hydrostatic pressure of the evolving fluid interface, rising of two bubbles, and square droplet deformation, and the effects of numerical parameters on simulation accuracy and stability are also discussed. Third, the integrated SPH model is applied to simulate molten droplet formation and dropping processes. The results show that an initial solid–liquid interface disappears during the melting process, and new liquid–liquid interfaces gradually form and evolve under the action of surface tension, gravity, and viscosity. Phenomena such as thin-layer fluid dynamics and capillary instabilities are also reproduced, showing the effectiveness of the model for handling multiphase flow with heat conduction and phase change.
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Favaro, Marco, Fatwa Abdi, Ethan Crumlin, Zhi Liu, Roel van de Krol, and David Starr. "Interface Science Using Ambient Pressure Hard X-ray Photoelectron Spectroscopy." Surfaces 2, no. 1 (January 28, 2019): 78–99. http://dx.doi.org/10.3390/surfaces2010008.
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The development of novel in situ/operando spectroscopic tools has provided the opportunity for a molecular level understanding of solid/liquid interfaces. Ambient pressure photoelectron spectroscopy using hard X-rays is an excellent interface characterization tool, due to its ability to interrogate simultaneously the chemical composition and built-in electrical potentials, in situ. In this work, we briefly describe the “dip and pull” method, which is currently used as a way to investigate in situ solid/liquid interfaces. By simulating photoelectron intensities from a functionalized TiO2 surface buried by a nanometric-thin layer of water, we obtain the optimal photon energy range that provides the greatest sensitivity to the interface. We also study the evolution of the functionalized TiO2 surface chemical composition and correlated band-bending with a change in the electrolyte pH from 7 to 14. Our results provide general information about the optimal experimental conditions for characterizing the solid/liquid interface using the “dip and pull” method, and the unique possibilities offered by this technique.
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McFadden, G. B., S. R. Coriell, L. N. Brush, and K. A. Jackson. "Interface Instabilities During Laser Melting of Thin Films." Applied Mechanics Reviews 43, no. 5S (May 1, 1990): S70—S75. http://dx.doi.org/10.1115/1.3120854.
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Thin silicon films on a cooled substrate are often found to develop two-phase lamellar structures upon radiative heating. Jackson and Kurtz developed a two-dimensional model for the process in which the heated film consists of alternating parallel bands of liquid and solid phases separated by straight solid-liquid interfaces. To understand the cellular or dendritic structures that sometimes are observed in these interfaces, they also performed a linearized morphological stability analysis and obtained the conditions for the growth or decay of infinitesimal perturbations to the interface. In this work we extend that analysis to finite amplitudes by developing a boundary integral representation of the thermal field, and obtain numerical solutions for nonplanar solid-liquid interfaces.
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Yu, C. J., G. Evmenenko, A. G. Richter, A. Datta, J. Kmetko, and P. Dutta. "Order in molecular liquids near solid–liquid interfaces." Applied Surface Science 182, no. 3-4 (October 2001): 231–35. http://dx.doi.org/10.1016/s0169-4332(01)00410-x.
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Magalhães e Silva, Diogo, Tânia Ribeiro, Luís C. Branco, Rogério Colaço, Amélia Gonçalves da Silva, and Benilde Saramago. "Hydrophobic ionic liquids at liquid and solid interfaces." Tribology International 129 (January 2019): 459–67. http://dx.doi.org/10.1016/j.triboint.2018.08.018.
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Divya, Velpula, and M. V. Sangaranarayanan. "Electrodeposition of Polymer Nanostructures using Three Diffuse Double Layers: Polymerization beyond the Liquid/Liquid Interfaces." Electrochemical Energy Technology 4, no. 1 (April 28, 2018): 6–20. http://dx.doi.org/10.1515/eetech-2018-0002.
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Abstract Nanostructured conducting polymers have received immense attention during the past few decades on account of their phenomenal usefulness in diverse contexts, while the interface between two immiscible liquids is of great interest in chemical and biological applications. Here we propose a novel Electrode(solid)/Electrolyte(aqueous)/Electrolyte(organic) Interfacial assembly for the synthesis of polymeric nanostructures using a novel concept of three diffuse double layers. There exist remarkable differences between the morphologies of the polymers synthesized using the conventional electrode/electrolyte method and that of the new approach. In contrast to the commonly employed electrodeposition at liquid/liquid interfaces, these polymer modified electrodes can be directly employed in diverse applications such as sensors, supercapacitors etc.
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Zachman, Michael J., Emily Asenath-Smith, Lara A. Estroff, and Lena F. Kourkoutis. "Site-Specific Preparation of Intact Solid–Liquid Interfaces by Label-Free In Situ Localization and Cryo-Focused Ion Beam Lift-Out." Microscopy and Microanalysis 22, no. 6 (November 21, 2016): 1338–49. http://dx.doi.org/10.1017/s1431927616011892.
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AbstractScanning transmission electron microscopy (STEM) allows atomic scale characterization of solid–solid interfaces, but has seen limited applications to solid–liquid interfaces due to the volatility of liquids in the microscope vacuum. Although cryo-electron microscopy is routinely used to characterize hydrated samples stabilized by rapid freezing, sample thinning is required to access the internal interfaces of thicker specimens. Here, we adapt cryo-focused ion beam (FIB) “lift-out,” a technique recently developed for biological specimens, to prepare intact internal solid–liquid interfaces for high-resolution structural and chemical analysis by cryo-STEM. To guide the milling process we introduce a label-free in situ method of localizing subsurface structures in suitable materials by energy dispersive X-ray spectroscopy (EDX). Monte Carlo simulations are performed to evaluate the depth-probing capability of the technique, and show good qualitative agreement with experiment. We also detail procedures to produce homogeneously thin lamellae, which enable nanoscale structural, elemental, and chemical analysis of intact solid–liquid interfaces by analytical cryo-STEM. This work demonstrates the potential of cryo-FIB lift-out and cryo-STEM for understanding physical and chemical processes at solid–liquid interfaces.
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Rettenmayr, Markus, Oleg Kashin, and Stephanie Lippmann. "Simulation of Liquid Film Migration during Melting." Materials Science Forum 790-791 (May 2014): 127–32. http://dx.doi.org/10.4028/www.scientific.net/msf.790-791.127.
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Melting of a single-phase polycrystalline material is known to start by the formation of liquid films at the surface and at grain boundaries. The internal liquid films are not necessarily quiescent, but can migrate to avoid/reduce supersaturation in the solid phase. The migration is discussed in the literature to be governed by coherency strains of the solid/liquid interface, by concentration gradients in the liquid or by concentration gradients in the solid phase. A phase transformation model for diffusional phase transformations considering interface thermodynamics (possible deviations from local deviations) has been put up to describe the migration of the solid/liquid (trailing) and the liquid/solid (leading) interfaces of the liquid film. New experimental results on melting in a temperature gradient in combination with simulation calculations reveal that concentration fluctuations in the liquid phase trigger the liquid film migration and determine the migration direction, until after a short time in the order of microseconds the process is governed by diffusion in the solid phase.
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Welland, M. E., S. O'Shea, A. W. McKinnon, and T. M. H. Wong. "Applications of AFM and STM: Solvation forces in liquids and inelastic photon excitation." Proceedings, annual meeting, Electron Microscopy Society of America 50, no. 2 (August 1992): 1156–57. http://dx.doi.org/10.1017/s0424820100130419.
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We describe here non-standard applications of scanned probe microscopy; one application making use of the force sensitivity of the AFM to measure solvation forces at the liquid-solid interface and the other application based on the STM where the tunnelling current is used to excite photon emission from a surface.An interesting aspect of the solid-liquid interface is the molecular order induced in the liquid by the solid surface. This order can give rise to observable changes in the short range forces acting between two solids in a liquid medium; so called “solvation” or “structural” forces. As a first investigation of the local variation of short range forces in liquids we have used an AFM to observe solvation forces near a graphite surface. The AFM is ideal for this work as it can typically measure very small forces (∼10-10N) with high lateral (∼0.3nm) and vertical resolution (∼0.03nm). In this study, an optical deflection type AFM is used in which the movement of a small cantilever is sensed by measuring the deflection of a laser beam focussed on the back of the lever.
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Agathopoulos, Simeon, D. U. Tulyaganov, and José Maria F. Ferreira. "Stages of Reactive Wetting." Key Engineering Materials 280-283 (February 2007): 1801–4. http://dx.doi.org/10.4028/www.scientific.net/kem.280-283.1801.
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A universal model for describing the wetting kinetics at solid/liquid interfaces, where interfacial chemical reaction occurs, is proposed, whereby four distinct stages separated from each other by transition points are anticipated. The stages are described by means of comparing the dimensions of the base of the liquid sessile drop with the evolution of the reaction product forming on the solid/liquid interface, over time.
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Lojkowski, Witold, Akira Otsuki, and Andrzej Morawski. "High-pressure effect on grain boundary wetting in aluminium bicrystals." International Journal of Materials Research 96, no. 10 (October 1, 2005): 1211–12. http://dx.doi.org/10.1515/ijmr-2005-0208.
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Abstract The effect of pressure and misorientation on grain boundary wetting in aluminium bicrystals has been investigated. The grain boundaries were of [100] symmetrical tilt type. The wetting liquid was an Sn– Zn alloy. It is shown that the wetting angle is a function of misorientation but not of pressure. The reasons of the above results are discussed, assuming a linear dependence between the interface energy and pressure. It is shown that the difference of energy of the liquid/solid and solid/solid interface as well as the misorientation dependence of energy is simply proportional to the free volume of the interfaces.
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Kawano, Satoyuki, Hiroyuki Hashimoto, Akio Ihara, and Keiji Shin. "Sequential Production of mm-Sized Spherical Shells in Liquid-Liquid Gas Systems." Journal of Fluids Engineering 118, no. 3 (September 1, 1996): 614–18. http://dx.doi.org/10.1115/1.2817804.
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A new device has been developed for sequential production of mm-sized solid spherical shells using liquid-liquid gas systems. This device comprises a cylindrical vessel, for containing two kinds of immiscible liquids, and a gas injection orifice, set at the center of the vessel’s bottom. Solid spherical shells are successfully and sequentially produced by solidifying rising liquid spherical shells, formed sequentially at the horizontal interface between two immiscible liquids.
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Quan, Jiliang, Guanzhen Ke, Yali Zhang, Jian Liu, and Jinqiang Huang. "Study on Growth Interface of Large Nd:YAG Crystals." Crystals 13, no. 6 (June 19, 2023): 970. http://dx.doi.org/10.3390/cryst13060970.
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A study was performed on the growth interface of a large-diameter 1 at% neodymium-doped yttrium aluminum garnet (Nd:YAG) single crystal grown using the Czochralski method. Red parallel light and an orthogonal polarizing system were used to observe the distribution of the central and lateral cores of the crystal at different growth interfaces. The solid–liquid interface of large-diameter Nd:YAG crystal growth was mainly determined via the interaction between natural and forced convection. The shape of the solid–liquid interface was mainly controlled via maintaining the crystal rotation rate and the temperature field. Interface inversion generally occurred during the shoulder-expanding stage and late stages of the growth of the cylindrical portion of the crystal. The occurrence of interface inversion is directly related to the temperature field, process parameters, and diameter of the crystal. The growth shape of the crystal interface determined the size and distribution of the central and lateral cores of the crystal. The area of the central and lateral cores was reduced via adjusting the temperature gradient of the solid–liquid interface and crystal rotation speed.
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Weinhardt, L., M. Blum, O. Fuchs, A. Benkert, F. Meyer, M. Bär, J. D. Denlinger, W. Yang, F. Reinert, and C. Heske. "RIXS investigations of liquids, solutions, and liquid/solid interfaces." Journal of Electron Spectroscopy and Related Phenomena 188 (June 2013): 111–20. http://dx.doi.org/10.1016/j.elspec.2012.10.006.
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Yan, Shuo, Ali Merati, Chae-Ho Yim, Elena Baranova, Arnaud Weck, and Yaser Abu-Lebdeh. "Understanding the Role of Liquid Electrolytes in Performance Improvement of Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 551. http://dx.doi.org/10.1149/ma2022-014551mtgabs.
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Abstract Garnet-type Li7La3Zr2O12 (LLZO) Solid-State Electrolytes (SSEs) enable Solid-State Lithium Metal Batteries (SSLMBs) with high power density due to their superior ionic conductivity over 1 mS cm-1 at room temperature and good chemical stability against Lithium (Li) metal. A major cause of failure in SSLMBs is the large interfacial resistance between LLZO and electrodes. The high resistance at the interfaces is normally associated with insufficient solid-solid surface contact. It is a common practice to introduce a Liquid Electrolyte (LE) in SSLMBs either in combination with SSEs to form quasi-solid electrolytes or as the interface to enhance battery cycling performance. Several studies are conducted on resolving the contact issue between LLZO and the Li-metal anode but very few focused on the LLZO/cathode interface. In this research, a carbonate-based LE was introduced at the interface of Li6.5La2.9Ba0.1Zr1.4Ta0.6O12 (LLBZTO) | LiNi0.6Mn0.6Co0.2O2 (NMC 622) cathode with the aim of understanding the mechanism which the LE enhances the SSLMBs performance, using the Scanning Transmission X-ray Microscopy (STXM) and X-ray Absorption Scanning (XAS). The assembled Li | LLBZTO SSEs | LE | NMC 622 cell exhibited an initial discharge capacity of 168 mAh g-1 with a capacity retention ratio of ~82 % after 30 cycles. The results from the STXM revealed the reactions of the LE with LLZO and NMC 622. The XAS analysis showed the formation of two new interfaces: Cathode-Electrolyte Interface (CEI) and Solid-Liquid Electrolyte Interface (SLEI). Also, the result indicated that the LE decomposed completely in the cell after 30 cycles and transformed to a dense and robust SLEI. This in turn led to the enhanced interfacial contact with the cathode and an improved Li+ ion transport at the interface. In addition, fluorides (i.e., LiF and LaF3) and carbonates (i.e., Li2CO3) were confirmed as the main components of the SLEI. In this study, two interfaces in SSLMBs (CEI and SLEI) were characterized. Fully understanding the roles of LE as the interface would enhance the practical application of quasi-solid electrolytes in SSLMBs. Keywords Solid-state lithium metal batteries; Garnet; Interface; Ceramic electrolyte; STXM
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Sun, Zhouting, Mingyi Liu, Yong Zhu, Ruochen Xu, Zhiqiang Chen, Peng Zhang, Zeyu Lu, Pengcheng Wang, and Chengrui Wang. "Issues Concerning Interfaces with Inorganic Solid Electrolytes in All-Solid-State Lithium Metal Batteries." Sustainability 14, no. 15 (July 25, 2022): 9090. http://dx.doi.org/10.3390/su14159090.
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All-solid-state batteries have attracted wide attention for high-performance and safe batteries. The combination of solid electrolytes and lithium metal anodes makes high-energy batteries practical for next-generation high-performance devices. However, when a solid electrolyte replaces the liquid electrolyte, many different interface/interphase issues have arisen from the contact with electrodes. Poor wettability and unstable chemical/electrochemical reaction at the interfaces with lithium metal anodes will lead to poor lithium diffusion kinetics and combustion of fresh lithium and active materials in the electrolyte. Element cross-diffusion and charge layer formation at the interfaces with cathodes also impede the lithium ionic conductivity and increase the charge transfer resistance. The abovementioned interface issues hinder the electrochemical performance of all-solid-state lithium metal batteries. This review demonstrates the formation and mechanism of these interface issues between solid electrolytes and anodes/cathodes. Aiming to address the problems, we review and propose modification strategies to weaken interface resistance and improve the electrochemical performance of all-solid-state lithium metal batteries.
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Nishi, Naoya, Naohiro Yoshida, Yishan Zhou, Yuko Yokoyama, and Tetsuo Sakka. "Electroless Deposition of Base Metals at the Liquid/Liquid Interface of Ionic Liquids." ECS Meeting Abstracts MA2023-02, no. 56 (December 22, 2023): 2714. http://dx.doi.org/10.1149/ma2023-02562714mtgabs.
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Metal nanostructures can be formed at the electrochemical liquid/liquid interface, so-called ITIES. Our group has presented a method to form metal nanostructures at the liquid/liquid interface between ionic liquid (IL) and water (W) [1-10]. This IL/W method utilizes the spatial selectivity of the reaction site only at the liquid/liquid interface, which is achieved by the separation of metal precursor ions dissolved in the W phase and reducing agent in the IL phase. The metal reduction reaction is regarded as the electron transfer across the IL/W interface, which enables us to analyze the reaction process with liquid-liquid electrochemistry at the IL/W interface [11]. Moreover, the usage of ILs (not molecular oils) leads to the formation of 1-dimensional (1D) nanostructures despite the inherent 2D geometry of the liquid/liquid interface, as a result of the structure-forming ability of ILs at the air [12-14], liquid [14-16], and solid [17-19] interfaces. By using this IL/W method, we have successfully prepared 1D nanostructures of noble metals such as Au [1,6], Ag [7], Pt [3], and Pd [5,6], and also their composites with polymer [2] and nanocarbons [8-10]. In this presentation, we would like to introduce our very recent efforts to develop a sister method that uses another liquid/liquid interface between IL and oil (O). Wet chemical techniques for the metal nanostructure formation in general, including our IL/W method described above, involve water and therefore cannot escape from the limitation of metal elements to noble ones. In contrast, the IL/O method [20-22] is water-free and therefore can be used even for base metals, expanding the applicability and versatility of wet chemistry for metal nanostructure formation. In the presentation, we introduce our water-free liquid/liquid interface method, the electrochemical measurements of the electron and ion transfers across the interface, and the obtained nanostructures of base metals such as zinc, aluminum, and magnesium. References Nishi, T. Kakinami, T. Sakka, Chem. Commun., 51 (2015) 13638. Nishi, I. Yajima, K. Amano, T. Sakka, Langmuir, 34 (2018) 2441. Zhang, N. Nishi, K. Amano, T. Sakka, Electrochim. Acta, 282 (2018) 886. Takagi, N. Nishi, T. Sakka, Chem. Lett., 48 (2019) 589. Zhang, N. Nishi, T. Sakka, ACS Appl. Mater. Interfaces, 11 (2019) 23731. Zhang, N. Nishi, T. Sakka, Electrochim. Acta, 325 (2019) 134919. Zhang, N. Nishi, T. Sakka, Colloids Surf. A, 597 (2020) 124747. Zhang, N. Nishi, I. Koya, T. Sakka, Chem. Mater., 32 (2020) 6374. Koya, T. Sakka, N. Nishi, Langmuir, 37 (2021) 9553. Koya, Y. Yokoyama, T. Sakka, N. Nishi, Chem. Lett., 51 (2022) 643. Kakiuchi and N. Nishi, Electrochemistry, 74 (2006) 942. Nishi, Y. Yasui, T. Uruga, H. Tanida, T. Yamada, S. Nakayama, H. Matsuoka, T. Kakiuchi, J. Chem. Phys., 132 (2010) 164705. Nishi, T. Uruga, H. Tanida, T. Kakiuchi, Langmuir, 27 (2011) 7531. Nishi, T. Uruga, H. Tanida, J. Electroanal. Chem., 759 (2015) 129. Katakura, K. Amano, T. Sakka, W. Bu, B. Lin, M. Schlossman, N. Nishi, J. Phys. Chem. B, 124 (2020) 6412. Ishii, T. Sakka, N. Nishi, Phys. Chem. Chem. Phys., 23 (2021) 22367. Nishi, J. Uchiyashiki, Y. Ikeda, S. Katakura, T. Oda, M. Hino, N. Yamada, J. Phys. Chem. C, 123 (2019) 9223. Nishi, T. Yamazawa, T. Sakka, H. Hotta, K. Hanaoka, H. Takahashi, Langmuir, 36 (2020) 10397. Nishi, J. Uchiyashiki, T. Oda, M. Hino, N. Yamada, Bull. Chem. Soc. Jpn., 94 (2021) 2914. Kuroyama, N. Nishi, T. Sakka, J. Electroanal. Chem., 881 (2021) 114959. Nishi, Y. Kuroyama, N. Yoshida, Y. Yokoyama, T. Sakka, ChemElectroChem, 10 (2023) e202201000. Yoshida, Y. Yokoyama, T. Sakka, N. Nishi, to be submitted.
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Cucinotta, Clotilde S. "(Invited) Towards a Realistic Modelling of Solid-Liquid Interfaces." ECS Meeting Abstracts MA2023-01, no. 30 (August 28, 2023): 1806. http://dx.doi.org/10.1149/ma2023-01301806mtgabs.
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In this talk I will introduce some issues connected with the simulation of electrified interfaces at the nanoscale focusing on simulating the effect of an applied potential to an electrode, using realistic models for the charged electrode electrolyte interface. I will present some recent progress in the simulation of the double layer of fundamental solid liquid interfaces of interest for corrosion and water splitting, and its response to changes of potential applied to the cell [1]; this is obtained applying a general ab initio electrode-charging approach we developed. [1] R. Khatib, A. Kumar, S. Sanvito, M. Sulpizi and C. S. Cucinotta*, The nanoscale structure of the Pt-water double layer under applied potential revealed, 2021, 391, 138875 In this talk I will introduce some issues connected with the simulation of electrified interfaces at the nanoscale focusing on simulating the effect of an applied potential to an electrochemical (EC) cell, using realistic models for the charged electrode electrolyte interface. I will present some recent progress in the simulation of the double layer of the fundamental solid liquid interfaces of interest for corrosion and water splitting and its response to changes of potential applied to the cell [1]; this is obtained applying a general ab initio electrode-charging approach we developed. [1] R. Khatib, A. Kumar, S. Sanvito, M. Sulpizi and C. S. Cucinotta*, The nanoscale structure of the Pt-water double layer under applied potential revealed, 2021, 391, 138875
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Zhang, Han Long, Yan Feng Han, Jun Wang, Yong Bing Dai, and Bao De Sun. "Grain Refinement Mechanism of Al-5Ti-1B Master Alloy by Ab Initio Calculations." Materials Science Forum 794-796 (June 2014): 746–51. http://dx.doi.org/10.4028/www.scientific.net/msf.794-796.746.
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To exactly understand the grain refining mechanism of α-Al by the Al-5Ti-1B master alloy, the structural properties of α-Al/solid-TiB2(S/S) and liquid-Al/solid-TiB2(L/S) interfaces were studied using the first-principles method. Different ordered structures were formed on the interfaces with different terminations of TiB2(0001) surface, which determines the nucleant potency of TiB2. The heterogeneous nucleation of α-Al on the B-terminated surface is frustrated by an AlB2-like structure formed at the interface. In contrast, a five-layer quasi-solid region with stacking sequence of fcc-Al (111) planes forms on the Ti-terminated TiB2(0001) surface, which is the basis of successful heterogeneous nucleation of α-Al. Moreover, when redundant Ti solute being added into the liquid Al region of Ti-terminated liquid-Al/TiB2interface, the quasi-solid Al region further extends until entire solidification. The reason for using the Al-5Ti-1B master alloy rather than TiB2powders as the commercial refiner in Al industry lies in two aspects: the excessive Ti atoms in the master alloy could guarantee sufficient Ti chemical potential to form Ti-terminated surface of TiB2, and the redundant Ti solute in inoculated melts could facilitate the growth of quasi-solid Al region at the solid/liquid interface.