Low-temperature Liquid Research Articles

Coupling ultrafine SiO2 nanoparticles with three-dimensional porous Ti3C2Tx MXene as anode materials for high-performance lithium-ion batteries

Silicon dioxide with high-capacity and abundant resource is regarded as a promising anode material for lithium-ion batteries, but the poor intrinsic electrical conductivity and large volume change during the discharge/charge cycles impede its practical application. Herein, a three-dimensional porous composite of Ti3C2Tx@SiO2 was fabricated with a low-temperature liquid phase method, and the ratio of SiO2 and Ti3C2Tx was regulated. The as-prepared A-MX@SiO2-2 with the optimal composition exhibits the best cycle performance (437.9 mAh g−1 after 1000 cycles at 0.1 A g−1) and rate performance (130.0 mA h g−1 at 2 A g−1), which are much higher than pure SiO2 and MXene. The excellent electrochemical performance can be ascribed to the synergistic effect of ultrafine SiO2 nanoparticles and three-dimensional porous Ti3C2Tx, which can shorten the Li+ transport pathway, accelerate electron transfer, and relieve the stress caused by the volume expansion of SiO2. The composite structure effectively inhibits both the aggregation of SiO2 and restacking of Ti3C2Tx. Furthermore, the in-situ formed SiO2 can firmly anchored on the surface of Ti3C2Tx nanosheet by robust interfacial bonding, which enhances the structural stability and conductivity. This research provides a feasible design strategy for synthesis of Ti3C2Tx@SiO2 composite to be employed as advanced energy storage materials.

CALCULATION OF THE ELECTRODE REACTION RATE ON A GRAPHITE CATHODE OF ALUMINUM-ION BATTERY WITH 1-ETHYL-3-METHYLIMIDAZOLIUM CHLORIDE

A method for determining the rate of sorption of chloraluminate complexes on graphite material as the main cathode reaction in aluminum-ion batteries with an ionic liquid as an electrolyte is proposed in terms of classic chemical kinetics approach. The method is applied to the description of the rate of a one-electron cathode reaction that is in the case the sorption/desorption of complexes on the electrode surface with no migration in the interlayer space of graphite taken into account. The experimental part is based on the selection and providing of measurement conditions and the ratio of the components of the cell to ensure that the rate of the cathode process sets the rate of current generation of the cell. The rate of supply/removal of electrons, as participants in the reaction, thus can be directly related to the reaction rate on graphite. The point of reaching the limiting current on the polarization curve in that case corresponds the limiting rate of the chemical sorption reaction. The approach takes into account the effect of other limiting processes, such as the rate of removal/supply of electrons, the rate of removal/supply of ions to/from the electrolyte volume, and the rate of anodic dissolution/deposition of aluminum. The calculated value of the reaction rate for graphite material grade EC-02 and low-temperature ionic liquid 1-ethyl-3-methylimidazole chloride in a mixture with aluminum chloride (1 : 1.3) was calculated to be 46 µmol/cm2 · s.

Surface tension effects on cryogenic liquid injection dynamics in supercritical environment

The injection of cryogenic fluids into environments where the prevailing conditions are supercritical in comparison to the critical point of the injected cryogenic fluid is encountered in cryogenic rocket engines, and novel engine architectures such as the recuperated split cycle engine. The physical characteristics of cryogens injected into supercritical environment are rather unclear. While surface tension is usually assumed to be absent/negligible for supercritical fluids, recent experimental research has identified the existence of surface tension and its effects on liquid hydrocarbons in supercritical environment. This research work proposes an alternative computationally simple adaptive surface tension algorithm for the simulation of a liquid injected into supercritical environment. The numerical simulations presented here correspond to single- and binary-specie cases of iquid nitrogen and liquid methane respectively, undergoing phase transition post their injection into supercritical conditions. Following a critical review of related numerical works, this paper begins with a brief explanation of the physics behind the surface tension effect in a binary-fluid interface in which a supercritical fluid is involved and we present why this effect is of relevance to supercritical cryogenic jets? Then, the rationale and specifics of the the new modelling framework based on adaptive surface tension is discussed along with its implications. The results of the numerical simulations of low-temperature vs near-critical temperature iquid nitrogen and liquid methane injection dynamics revealed the drastically different fluid- and thermo-dynamics at play in these two cases. The role of surface tension at these conditions is also explored.

Electroforming as a Novel One-Step Manufacturing Method of Structured Aluminum Foil Current Collectors for Lithium-Ion Batteries

Conventionally, cathode current collectors for lithium-ion batteries (LIB) consist of an aluminum foil generally manufactured by a rolling process. In the present work, a novel one-step manufacturing method of structured aluminum foil current collectors for lithium-ion batteries by electroforming is introduced. For this, a low-temperature chloride-based ionic liquid was used as an electrolyte and a rotating cylinder out of stainless steel as a temporary substrate. It was shown that the structure of the aluminum foils can be adjusted from dense and flat to three-dimensional by choosing an appropriate substrate rotation speed and current density. Scanning electron microscopy (SEM) and white light interferometry (WLI) were utilized to analyze the foils’ surface morphology, structure and topography. The SEM analysis of the aluminum foils showed that the rolling process produced a foil with small grains, while electrodeposition resulted in foils with different degrees of grain growth and seed formation. This was in total agreement with WLI results that revealed significant differences in terms of roughness parameters, including the peak-to-valley difference Rpv, the root-mean-square roughness Rq and the arithmetic mean roughness Ra. These were, respectively, equal to 6.8 µm, 0.35 µm and 0.279 µm for the state-of-the-art foil and up to 96.6 µm, 10.92 µm and 8.783 µm for the structured electroformed foil. Additionally, cyclic voltammetry (CV) of the aluminum foils was used to investigate their passivation behavior within the typical LIB cathode potential operation window. The strong decrease in the current density during the second cycle compared to the first cycle, where an anodic peak appeared between 4.0 and 4.4 V vs. Li/Li+, demonstrated that passivation occurs in the same manner as observed for commercial Al current collectors.

Spatially Resolved Structural Order in Low-Temperature Liquid Electrolyte.

Spatially Resolved Structural Order in Low-Temperature Liquid Electrolyte.

Four-Dimensional Printing of Temperature-Responsive Liquid Crystal Elastomers with Programmable Shape-Changing Behavior.

Liquid crystal elastomers (LCEs) are polymer networks that exhibit anisotropic liquid crystalline properties while maintaining the properties of elastomers, presenting reversible high-speed and large-scale actuation in response to external stimuli. Herein, we formulated a non-toxic, low-temperature liquid crystal (LC) ink for temperature-controlled direct ink writing 3D printing. The rheological properties of the LC ink were verified under different temperatures given the phase transition temperature of 63 °C measured by the DSC test. Afterwards, the effects of printing speed, printing temperature, and actuation temperature on the actuation strain of printed LCEs structures were investigated within adjustable ranges. In addition, it was demonstrated that the printing direction can modulate the LCEs to exhibit different actuation behaviors. Finally, by sequentially conforming structures and programming the printing parameters, it showed the deformation behavior of a variety of complex structures. By integrating with 4D printing and digital device architectures, this unique reversible deformation property will help LCEs presented here apply to mechanical actuators, smart surfaces, micro-robots, etc.

Evaluating the Performance of Low-Temperature Liquid Separation Devices with Two-Stage Refrigeration and Pre-Cooling

Evaluating the Performance of Low-Temperature Liquid Separation Devices with Two-Stage Refrigeration and Pre-Cooling

Low-Temperature Transient Liquid Phase Bonding Technology via Cu Porous-Sn58Bi Solid–Liquid System under Formic Acid Atmosphere

This study proposes a low-temperature transient liquid phase bonding (TLPB) method using Sn58Bi/porous Cu/Sn58Bi to enable efficient power-device packaging at high temperatures. The bonding mechanism is attributed to the rapid reaction between porous Cu and Sn58Bi solder, leading to the formation of intermetallic compounds with high melting point at low temperatures. The present paper investigates the effects of bonding atmosphere, bonding time, and external pressure on the shear strength of metal joints. Under formic acid (FA) atmosphere, Cu6Sn5 forms at the porous Cu foil/Sn58Bi interface, and some of it transforms into Cu3Sn. External pressure significantly reduces the micropores and thickness of the joint interconnection layer, resulting in a ductile fracture failure mode. The metal joint obtained under a pressure of 10 MPa at 250 °C for 5 min exhibits outstanding bonding mechanical performance with a shear strength of 62.2 MPa.

Liquid phase sintering of Nb doped SrTiO3-δ ceramics with enhanced thermoelectric figure of merit

SrTiO3 (STO) based ceramics are a promising n-type semiconductor oxide for high-temperature thermoelectric application. In the present work, the results of liquid-phase sintering (LPS) aid incorporating various concentrations of Al2O3, CuO and ZnOin Nb-doped STO (STN) is presented. With the inclusion of sintering aid, densities comparable to those obtained by conventional sintering (greater than 97%) were achieved for samples sintered as low as 1623 K. We also report the effect of various sintering aid (Al2O3, CuO, and ZnO) with different concentrations (1–5 wt %) on the thermoelectric figure of merit ZT of Nb-doped SrTiO3 (STN) ceramics. SEM images provided evidence of the presence of the low-temperature liquid phase around the grain boundaries of STN ceramics. The dislocations caused by liquid phase formation remove densification issues and enhances thermoelectric properties. A simultaneous increase in both electrical conductivity and the Seebeck coefficient was observed when the sintering aid concentration increased. The maximum electrical conductivity value of 390 Scm−1 at 420 K was obtained for the 5 wt % CuO added STN (STNCu5) ceramics, which was about two orders higher than the pristine STN sample sintered at that temperature. The highest PF value of 1040 Wm−2K−2 resulted in a remarkable ZT value of ≈0.4 (0.38) at 573 K for 5 wt % Al2O3 added STN (STNAl5) ceramics at a very low sintering temperature. To our knowledge, the LPS strategy is a completely novel approach in STO-based ceramics for thermoelectric applications.

Structural evolution of dendritic-structured Mg0.01V2O5 film electrodes of lithium-ion batteries during cycling

The development of viable high-capacity cathode materials is still a challenge for lithium-ion batteries (LIBs). In this work, Mg0.01V2O5 films with an interesting dendritic structure were grown in-situ on indium-tin oxide (ITO) conductive glass by a low temperature liquid phase deposition. The results exhibited the morphologies and properties of film electrodes were greatly affected by different annealing temperature. Among them, the Mg0.01V2O5 film electrode annealed at 450 °C showed the best electrochemical performance. It provided a high-capacity of 164.7 mA h m−2, and 141.2 mA h m−2 after 100 cycles that capacity retention of 85.7% at 176 mA m−2 in the LIB system. In addition, good cycling stability and rate performance were also impressive. The mechanism of Li+ insertion and extraction in the film electrode Mg0.01V2O5 was investigated by analyzing the phase evolution, lattice deformation, and elementary composition and valence of the film electrode after enduring electrochemical cycles. The insertion of Li+ in the interlayer allowed the creation of a new phase and the different diffusion rate of Li+ in the (010) crystal plane of the main phase, which caused the splitting behavior of the X‑ray diffraction peaks of this crystal plane. Encouragingly, it was the new phase produced during the cycle that worked with the principal phase, improving the diffusion kinetics and enhancing the electrochemical properties of LIBs. This work may provide a promising strategy to improve performance for LIBs.

Spatially resolved structural order in low-temperature liquid electrolyte.

Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiPF6) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at -30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high-salt concentration domains of the liquid electrolyte from liquid phase separation at the low temperature. Molecular dynamics simulations suggest the SRO originates from the Li+-(PF6-)n (n>2) local structural order induced by high LiPF6 salt concentration.

Enhanced thermoelectric performance in Bi0.5Sb1.5Te3/SiC composites prepared by low-temperature liquid phase sintering

A low-temperature liquid phase sintering method combined with post heat treatment was employed to prepare p-type Bi0.5Sb1.5Te3/SiC composites with enhanced thermoelectric properties.

Electrode processes in a deep eutectic solvent containing dissolved chromium(III) chloride

We considered the kinetics of electrochemical processes occurring during electrodeposition of coatings from a low-temperature ionic liquid based on a eutectic mixture of choline chloride and ethylene glycol, in which a trivalent chromium salt is dissolved. Irreversible current waves of Cr(III) ions discharge on a glassy carbon electrode in the electrolytes of studied compositions are not described by the "classical" equations of linear and cyclic voltammetry, which is due to both the presence of the migration component of the current and the cathodic passivation of the electrode. It has been established that the introduction of additional water into the electrolyte leads to an increase in the current density of the wave of irreversible discharge of Cr(III) ions on the glassy carbon electrode, which is caused by a significant decrease in the viscosity of the solution. The current efficiency of the chromium deposition reaction decreases when water is introduced into the ionic liquid. The X-ray amorphous coatings electrodeposited from the electrolyte under study, along with chromium, contain carbon and oxygen, the inclusion of which is due to the electrocatalytic properties of the freshly deposited chromium surface.

Mn2+ doped AgInS2 photocatalyst for formaldehyde degradation and hydrogen production from water splitting by carbon tube enhancement

In this work, AgInS2 and Mn2+ doped AgInS2 (Mn-AgInS2) with different Mn2+: (Ag++In3+) ratios were synthesized via a low temperature liquid method. The photocatalytic activity of the obtained samples was followed by taking formaldehyde as the target pollutant under visible light irradiation. The photocatalysts were passed through various characterization procedures to investigate their morphological, structural and photophysical characteristics. The optimal proportion sample [with the ratio n (Mn2+): n (Ag++In3+)=1:100] photodegraded about 79% formaldehyde in 150min. These upgraded activities are attributed to the enhanced visible light absorption and superior charge separation due to the presence of Mn2+ as confirmed site from charge separation measurements. In addition, a possible mechanism for the photodegradation of formaldehyde is proposed based on the experimental results. Furthermore, the photocatalytic water splitting performance of Mn-AgInS2 and multi-walled carbon nanotubes (MWCNTs) modified Mn-AgInS2 is investigated and compared under simulated sunlight irradiation, and remarkable hydrogen production is achieved (105μmolh-1 g-1) by using the latter.

Adaptive reversible composite-based shape memory alloy soft actuators

This research demonstrates how a combination of two-way shape memory alloy (SMA), low-temperature liquid epoxy cure composites, and fibre reinforced plastic (FRP) may be utilised to create a novel reversible actuator with built driven functionality. The novelty of this work is that the actuator can reverse its original shape and be mounted on different customized structures. The strategy is based on a knowledge of SMA wires and the manufacturing principle underlying composite structure, as well as experiments to see how soft SMA-FRP can be programmed to bend. The folding mechanism is studied in terms of fabrication factors such as SMA training and strong interfacial bonding between SMA and epoxy resin, which influence the programming process and shape change. The two-way SMA wires are trained using the pre-straining method to programme the SMAs. The technique has been used to assemble the SMA wires with bond reliability to enhance the actuator interface's thermal behaviour. The SMA elements are directly inserted into FRP strips and epoxy resin is used as an adhesive, resulting in dynamic hybrid composites. The module is actuated using an electrical board with a current value between 3 and 6 A. The robustness, controllability, mechanical properties, and 500 life cycles of the actuator are tested. Results indicate a bending angle of 58° with 30 mm of deflection in 7 s after actuating the module. Also, 3D printing is used to print a gripper inspired by human fingers and a structure to lift various weights. The actuator’s performance as a soft gripper is reliable in terms of grasping objects of different shapes. • Fabricating a novel fast responsive composite-based shape memory alloy actuator. • Developing reversible SMA-FRP soft actuators which can be mounted on various designs. • Adjusting current intensity and FRP/epoxy resin thickness, soft actuators demonstrated electrically reversible bending. • Programming of two-way shape memory alloy wires. • Grasping/release is achieved in an electrically-actuated gripper by 3D-printed structures.

Spirulina (Arthrospira platensis) Extract Promotes Motility, Microscopic, and Antioxidative Parameters of Ram Semen during Refrigerated Storage

This study investigated the effect of spirulina ethanolic extract (SEE) on the quality of ram semen during low-temperature liquid storage and the relationship between sperm features. Ejaculates were collected from five Djallonké rams, pooled, extended with Tris-egg yolk (TEY) enriched with 0 (control), 20 (SEE20), 40 (SEE40), and 80 µg/mL (SEE80) of SEE to reach the concentration of 200×106 spz/mL, and stored at 4 °C for 72 h. Extended semen samples were assessed for total motility, progressive motility, sperm motion characteristics, viability, membrane integrity, and morphology at 6, 24, 48 and 72 h of storage. Moreover, malondialdehyde (MDA), nitric oxide (NO), superoxide dismutase, (SOD) and catalase (CAT) levels were measured at 72 h of storage. The enrichment of TEY with SEE at 40 and 80 µg/mL, improved sperm total motility at 48 and 72 h of storage (P

Effect of cobalt doping on the photocatalytic performance of AgInS2 for organic pollutant degradation and hydrogen production

In this work, AgInS2 (AIS) and cobalt (Co) doped AgInS2 (Co-AIS) are prepared by low-temperature liquid phase method using thioglycolic acid (TGA) as the stabilizing agent. The crystal structure, surface elements, binding energy, particle morphology, and optical properties of AIS and Co-AIS are analyzed by XRD, XPS, SEM, TEM, UV-Vis-DRS, and PL. Rhodamine B (RhB) and 4-nitrophenol (4-NP) are used as the model pollutants for evaluating the photocatalytic activities of AIS and Co-AIS. The optimal doping ratio of CoːIn is found to be 10.7:6.3. And, under this optimal ratio, Co-AIS can degrade 95 % of RhB in 1.5 h or 76 % of 4-NP in 2.5 h, respectively. The photocatalytic mechanism is proposed based on the active species trapping experiment, EPR technique, optical properties characterization, and the flat-band potential determination. Moreover, the photocatalytic water splitting performance of Co-AISs with or without the modification of the multi-walled carbon nanotubes (MWCNTs) are investigated, and remarkable hydrogen production is achieved. This research will open a new gateway to synthesizing AgInS2-based materials and exploring their photocatalytic activities.

Effect of Fragmentation on Pore Structures and Fractal Characteristics of Intact Coal and Deformed Coal Based on Experiments

Coal mining has to develop to deeper strata with the increasing demand for coal, which leads to frequent coal and gas outburst disasters. Especially, when there is a deformed coal in the coal seam, the outburst disasters are easier and more intense. Coal and gas outburst disasters can be promoted by the fragmentation. In order to clearly explain the reasons for the impact of fragmentation on deformed coal and gas outburst, mercury intrusion porosimetry, low-temperature liquid N2 adsorption test, and scanning electron microscope were carried out in this paper. The differences in pore characteristics of intact coal and deformed coal under different particle size conditions were analyzed from pore shapes, pore size distributions, and fractal dimensions. The damage paths of fragmentation on various kinds of pores in intact coal are as follows: macropores, mesopores, minipores, and micropores, and those on various kinds of pores in deformed coal are as follows: macropores, micropores, mesopores, and minipores. According to the fractal dimension theory and experimental results, the calculative results of fractal dimensions show that the fragmentation and tectonism reduce the surface roughness and structural complexity of macropores and mesopores and increase those of minipores and micropores in deformed coal. Finally, combined with the coupling effect of fragmentation and tectonism on pores, the reason of deformed coal with high crushing degree in fields of outburst was explained. The research provides the basis for the prevention of coal and gas outburst.

Cover Picture: 4‐Amino‐1‐Butyl‐1,2,4‐Triazolium Dinitramide – Synthesis, Characterization and Combustion of a Low‐Temperature Dinitramide‐Based Energetic Ionic Liquid (EIL) (Prop., Explos., Pyrotech. 7/2022)

The cover image is based on the Research Article 4-Amino-1-Butyl-1,2,4-Triazolium Dinitramide – Synthesis, Characterization and Combustion of a Low-Temperature Dinitramide-Based Energetic Ionic Liquid (EIL) by Uwe Schaller et al. https://doi.org/10.1002/prep.202200054.

ZrO2 and MxOy (M= La, Ce, and Nb) synergistically reinforced porous cordierite ceramics synthesized via a facile solid-state reaction

In an attempt to enhance the sintering and mechanical performance of porous cordierite ceramics (Mg2Al4Si5O18) as support materials for vehicle exhaust catalysts, ZrO2 and MxOy (M = La, Ce, and Nb) were simultaneously introduced into cordierite sintered at 1350 °C for 4 h. Then, the reinforced function of ZrO2 and MxOy on the properties of porous cordierite ceramics was systematically evaluated, especially for the sample co-doped with ZrO2 and La2O3. The results displayed a distinct enhancement in mechanical and thermal performance, and the cold compressive strength increased from 72.74 to 158.59 MPa as well as thermal conductivity ranged from 1.66 to 2.01 W m−1 K−1, respectively. It is found that ZrO2 facilitated activation sintering introduced via lattice distortion in cordierite and La2O3 accelerated the formation of cordierite and ZrSiO4 microcrystalline through the low-temperature liquid phase. The synergic effect between ZrO2 and La2O3, therefore, had a significant role in the reinforced mechanical and thermal performance of porous cordierite ceramics. This work not only offers a feasible strengthening strategy, but also expands the possibilities for building high-performance structural and functional ceramics.