Low-temperature Glass Research Articles

A fabrication of universal multifunctional coating with excellent adhesion on the surface of solid rocket motor insulation materials through a surface activation strategy based on multiple interaction forces

In this work, a novel universal multifunctional coating for insulation materials was prepared by using polyethyleneimine as the coating substrate, low-temperature molten glass powders and MXene as additives. Meanwhile, the universal coating was tightly adhered to the surface of the insulation materials through a surface activation strategy based on the synergistic effects of hydrogen bonding, electrostatic adsorption, and chemical bonding. The shear strength data showed that the adhesion between the universal coating and the three types of insulation material were higher than that of most commercial adhesives. In the case of EPDM, for example, the adhesion of the coating is 4.17 (epoxy glue), 1.04 (chemlok) and 1.67 (Neoprene) times that of commercial adhesives, respectively. In addition, the universal coating showed good heat resistance and thermal insulation, and formed a complete and dense char on the surface after exposure to flame. The maximum mass loss temperatures of the three coated insulation materials were 2.8, 6.5, and 9.3°C higher than the original samples, respectively. Thermal insulation tests showed that the coated insulation materials reduced the average top surface temperature by 29.68%, 40.84% and 29.06%, respectively, compared to the original samples. The results of anti-migration tests showed that the prepared universal coatings displayed generally superior anti-migration properties to the insulation materials, with equilibrium migration concentrations reduced by up to more than 80% compared to the original samples, which is better than the previous products of the same type. In addition, the application potential of the advanced multifunctional insulation materials obtained from the preparation was evaluated, resulting in an increase of more than 35% in peel strength and more than 20% in shear strength for all insulation materials with propellants. This work provides a simple and environmentally friendly generalized strategy to develop high performance insulation materials for aerospace fields.

Low-Temperature and High-Rate Rechargeable Aluminum Batteries Enabled by Ternary Eutectic Electrolytes.

Rechargeable aluminum batteries (RABs) have garnered extensive scientific attention as a promising alternative chemistry due to the inherent advantages associated with aluminum (Al) metal anodes, including their high theoretical capacities, cost-effectiveness, environmental friendliness, and inherent non-flammable properties. Nonetheless, the practical energy density of RABs is constrained by the electrolytes that support lower operational voltage windows. Herein, we report a ternary eutectic electrolyte composed of 1-ethyl-3-methylimidazolium chloride ([C2C1im]Cl):1-butyl-3-methylimidazolium chloride ([C4C1im]Cl):aluminum chloride (AlCl3) for the application of RABs. The electrolyte exhibits a high operational potential window (~3V vs. Al/Al3+ on SS 316) and high ionic conductivity (~8.3 mS.cm-1) while exhibiting only a low temperature glass transition at -65 oC suitable for all-climate conditions. Al||graphene nanoplatelets cell delivers a high capacity of ~117 mAh/g, and ~43 mAh/g at a very high current densities of 1A/g and 5A/g, respectively. The cells render a reversible capacity of 20 mAh/g at -20 oC and 17 mAh/g at -40 oC, indicating their suitability for operation under extreme environmental conditions. We comprehensively evaluated the design and optimization of carbon paper-based battery systems. The ternary eutectic electrolyte demonstrates exceptional electrochemical performance, thus signifying its substantial potential for utilization in high-performance energy storage systems in all climates.

Surface modification of dental zirconia implants with a low infiltration temperature glass.

The glass infiltration technique was employed for surface modification of zirconia implants in this study. The prepared glass-infiltrated zirconia with low infiltrating temperature showed excellent mechanical properties and enough infiltrating layer. The zirconia substrate was pre-sintered at 1,200°C and the glass infiltration depth reached 400 μm after infiltrating at 1,200°C for 10 h. The infiltrating glass has good wetting ability, thermal expansion match and good chemical compatibility with the zirconia substrate. Indentation fracture toughness and flexural strength of the dense sintered glass-infiltrated zirconia composite are respectively 5.37±0.45 MPa•m1/2 and 841.03±89.31 MPa. Its elasticity modulus is 163.99±7.6 GPa and has about 500 μm infiltrating layer. The glass-infiltrated zirconia can be acid etched to a medium roughness (1.29±0.09 μm) with a flexural strength of 823.65±87.46 MPa, which promotes cell proliferation and has potential for dental implants.

Study on the Effects of Organic Bonding Agent and Low-Temperature Glass Solder Process on the Performance of Compact Packaged Fiber Optic Temperature Sensors

Study on the Effects of Organic Bonding Agent and Low-Temperature Glass Solder Process on the Performance of Compact Packaged Fiber Optic Temperature Sensors

Room temperature imprinting of water-based microparticulate inks for realizing glass microfluidic channels

The combination of imprinting and extrusion overprinting of composite glass materials offers a pathway for the fabrication of fully integrated functional microfluidic devices. Utilizing novel low-temperature phosphate glasses, originally developed for 3D extrusion printing, imprinting now has been achieved with soft stamps. The current hybrid process demonstrates superior resolution compared to previously reported extrusion techniques, presenting possibilities for applications such as open microfluidic channels that can subsequently be sealed by extrusion printing. The water-based microparticle glass-ink enables patterning at room temperature and its solidification occurring through water evaporation within the glass particle scaffold. Following the demolding, sintering is conducted at a temperature of 485 °C, resulting in dense glass elements with porosity levels below 1 %. For straightforward microfluidic channel structures featuring channels ranging from 100-200 µm in width, the shape is fully preserved during demolding and sequential annealing. The shrinkage observed is almost isotropic. The channels were successfully tested in an open microfluidic setup and initial tests were performed with the closed channels.

Effect of TeO2 on sintering behavior and properties of B2O3-BaO-ZnO-SiO2-Al2O3 glass

The research on low-temperature lead-free glass is of great significance for the miniaturization, integration and intelligence of current electronic products, as well as environmental protection. In this article, we report the preparation of low-temperature lead-free B2O3-BaO-ZnO-SiO2-Al2O3-TeO2 glasses by a melt-quenching technique. With the increase of TeO2 content in glass, the glass transition temperature and melting temperature of sintered glass powder decrease, while its wettability and acid corrosion resistance show an increasing trend. The application of glass powder in the sintering experiment of terminal electrode slurry further proves this viewpoint. Compared with the poor sintering performance of the slurry with TeO2-free glass powder, the slurry containing TeO2 glass powder forms a very dense sintered solid, and the sintered slurry is tightly bonded to the ceramic substrate.

Low-temperature cluster spin glass transition in the single-domain NiCr2O4 nanoparticles

NiCr2O4 nanoparticles with average particle size ∼15 nm, a single-domain size maintains the bulk canted antiferromagnetic ground state, were synthesized by a microwave combustion method. The magnetic behavior was carefully investigated by static and dynamic magnetic susceptibility measurements. In addition to a spin-glass-like behavior below paramagnetic-ferrimagnetic transition at T C, the NiCr2O4 nanoparticles demonstrate a low-temperature cluster spin glass transition below the spin canting transition T S, which manifests itself as a magnetic anomaly peak around ∼12 K (at 100 Oe) in the zero-field cooled magnetization with a relatively stronger field dependence in a ‘de Almeida-Thouless’ line for spin glasses. The AC susceptibility analyses in different approaches demonstrate a larger relative peak temperature variation per frequency decade and a longer characteristic relaxation time in the order of 0.04 and 10−7 s, against 0.01 and 10−9 s for the high-temperature blocking, indicating the slow spin dynamics for the low-temperature cluster glassy phase. A field-temperature magnetic phase diagram is proposed for the single-domain NiCr2O4 nanoparticles.

The Harmonic and Gaussian Approximations in the Potential Energy Landscape Formalism for Quantum Liquids.

The potential energy landscape (PEL) formalism has been used in the past to describe the behavior of classical low-temperature liquids and glasses. Here, we extend the PEL formalism to describe the behavior of liquids and glasses that obey quantum mechanics. In particular, we focus on the (i) harmonic and (ii) Gaussian approximations of the PEL, which have been commonly used to describe classical systems, and show how these approximations can be applied to quantum liquids/glasses. Contrary to the case of classical liquids/glasses, the PEL of quantum liquids is temperature-dependent, and hence, the main expressions resulting from approximations (i) and (ii) depend on the nature (classical vs quantum) of the system. The resulting theoretical expressions from the PEL formalism are compared with results from path-integral Monte Carlo (PIMC) simulations of a monatomic model liquid. In the PIMC simulations, every atom of the quantum liquid is represented by a ring-polymer. Our PIMC simulations show that at the local minima of the PEL (inherent structures, or IS), sampled over a wide range of temperatures and volumes, the ring-polymers are collapsed. This considerably facilitates the description of quantum liquids using the PEL formalism. Specifically, the normal modes of the ring-polymer system/quantum liquid at an IS can be calculated analytically if the normal modes of the classical liquid counterpart are known (as obtained, e.g., from classical MC or molecular dynamics simulations of the corresponding atomic liquid).

Temperature measurement of molten glass under batch feeding process by means of electrical resistance tomography

Electrical Resistance Tomography stands out as a powerful tool applicable to opaque environments, particularly in scenarios involving highly contaminated flows, gas–liquid two-phase flows with elevated void fractions, and electrically-conductive fields. The semi-conductive nature of high-temperature molten glass renders resistance tomography suitable for determining temperature distributions within such optically opaque mediums. This study aims to extend the application of the tomography technique to the spatial measurement of temperature in high-temperature molten glass. In order to verify the effectiveness of the developed system, a preliminary test was conducted by using an electrolyte solution in water to explore the overall system capabilities. Following the confirmation of the effective resolution of the proposed system, the measurement apparatus was employed for the actual temperature measurement of molten glass. The developed equipment featured sixteen independent electrodes, a low-impedance multiplexer, amplifier, rectifier, and a oscillating signal generator. Electrical potentials of the electrodes were recorded using a high-impedance amplifier as well as a data logging system. Upon collecting the electrical potential dataset, reconstruction computations were executed using the software. The measurement results show that the developed measurement system facilitates the acquisition of quantitative temperature distributions, as evidenced by the injection of a batch of low-temperature glass beads.

Functionalization of Phosphate and Tellurite Glasses and Spherical Whispering Gallery Mode Microresonators.

Active whispering gallery mode resonators made as spherical microspheres doped with quantum dots or rare earth ions achieve high quality factors and are excellent candidates for biosensors capable of detecting biomolecules at low concentrations. However, to produce quantum dot-doped microspheres, new low melting temperature glasses are sought, which require surface functionalization and antibody immobilization for biosensor development. Here, we demonstrate the successful functionalization of three low melting point glasses and microspheres made of them. The glasses were made from sodium borophosphate, sodium aluminophosphate, and tellurite, and then, they were functionalized using (3-glycidyloxypropyl)trimethoxysilane in ethanol- and toluene-based protocols. Proper silanization was confirmed by energy-dispersive X-ray spectroscopy and fluorescence microscopy of an amino-modified luminescent oligonucleotide probe. Fluorescence imaging showed successful silanization for all tested samples and no degradation for aluminophosphate and tellurite glasses. The strongest signal was registered for tellurite glass samples functionalized using the toluene-based silanization protocol. This conclusion implies that this functionalization method is the most efficient and is highly recommended for future antibody immobilization and biosensing application.

Low-temperature fusion bonding of aluminosilicate glass via intermediate water

Aluminosilicate glass holds significant importance across various applications including display screens, medical devices, and the aerospace industry, owing to its excellent optical properties, superior strength, and chemical resistance. Compared with frequently used high-temperature fusion bonding, low-temperature direct glass bonding, with its potential for reliable, non-damaging fabrication of glass-based devices, is highly promising. However, achieving aluminosilicate glass bonding at a low temperature has remained a challenge due to its inherent chemical stability. This paper proposes a novel low-temperature fusion bonding method using a standard cleaning recipe assistant with intermediate water, resulting in bonding strength exceeding 10 MPa and optical transmittance surpassing 90 % at a moderate annealing temperature of 200 °C. Through surface and interface characterization, the role of water intermedia and bonding mechanism is analyzed and declared. The water trapped in the bonding interface reacts with the glass and lowers the glass transition temperature (Tg), softening the glass and filling the nanoscale gaps to further increase the bonding area in the low-temperature annealing process. Consequently, a continuous bonding interface is established, contributing to robust bonding strength and avoiding optical loss. Finally, this method is further demonstrated through the successful bonding of the glass with grating structures showing great optical properties. Notably, in contrast to traditional fusion bonding, this low-temperature fusion bonding method will not destroy the microstructures in the devices. This bonding strategy paves the way for the applications of aluminosilicate glass.

Nanoprinting low-temperature glass

Nanoprinting low-temperature glass

Emerging exotic compositional order on approaching low-temperature equilibrium glasses

The ultimate fate of a glass former upon cooling has been a fundamental problem in condensed matter physics and materials science since Kauzmann. Recently, this problem has been challenged by a model with an extraordinary glass-forming ability effectively free from crystallisation and phase separation, two well-known fates of most glass formers, combined with a particle-size swap method. Thus, this system is expected to approach the ideal glass state if it exists. However, we discover exotic compositional order as the coexistence of space-spanning network-like structures formed by small-large particle connections and patches formed by medium-size particles at low temperatures. Therefore, the glass transition is accompanied unexpectedly by exotic compositional ordering inaccessible through ordinary structural or thermodynamic characterisations. Such exotic compositional ordering is found to have an unusual impact on structural relaxation dynamics. Our study thus raises fundamental questions concerning the role of unconventional structural ordering in understanding glass transition.

Heat-Seal Ability and Fold Cracking Resistance of Kaolin-Filled Styrene-Butadiene-Based Aqueous Dispersions for Paper-Based Packaging

Dispersion coatings are offered as alternative solutions to extrusion coating technology for paper-based packaging. In addition to providing barrier properties, waterborne dispersions may implement the processing and converting properties of coated substrates, which are of extreme interest for an effective transfer to the industry. In this work, styrene-butadiene-based aqueous dispersions were formulated considering different amounts of kaolin as pigment. The authors assessed the heat-seal ability, fold cracking resistance, and blocking tendency, comparing the results against commercial dispersion coating grades. Kaolin content dominated the sealing behavior of experimental formulations, changing the minimum heat-seal temperature from 80 °C to >140 °C for 0% and 60% kaolin solid content, respectively. On the contrary, commercial grades were mostly affected by temperature. Additionally, despite the low latex glass temperature (0 °C), experimental formulations generally showed little, if any, blocking. On the downside, increasing kaolin content eases fold cracking, showing a different magnitude according to fold direction and coat orientation yet achieving a higher moisture barrier compared to commercial grades for both folded and unfolded samples.

Low-Temperature Fluoro-Borosilicate Glass for Controllable Nano-Crystallization in Glass Ceramic Fibers.

A fluorosilicate (FS) nano-crystallized glass ceramic (NGC) is one of the most commonly used gain materials for applications in optical devices due to its excellent thermal stability as well as high-efficiency luminescence. However, FS glass can hardly be used to prepare NGC fibers due to its high preparation temperature. Here, a series of low-temperature fluoro-borosilicate (FBS) glasses were designed for the fabrication of active NGC fibers. By modulating B2O3, the preparation temperature of FBS glass was reduced to 1050 °C, and the crystallization in FBS NGCs was more controllable than in FS NGC. The crystallization of the impure phase was inhibited, and single-phase rare earth (RE)-fluoride nanocrystals were controllably precipitated in the FBS NGCs. The 40Si-20B FBS NGC not only exhibited a higher optical transmittance, but the luminescence efficiency was also much higher than traditional FS NGCs. More importantly, NGC fibers were successfully fabricated by using the designed FBS glass as core glass. Nanocrystals were controllably precipitated and greatly enhanced, and upconversion luminescence was observed in NGC fibers. The designed FBS NGCs provided high-quality optical gain materials and offered opportunities for fabricating a wide range of NGC fibers for multiple future applications, including fiber lasers and sensors.

Universality of stringlet excitations as the origin of the boson peak of glasses with isotropic interactions

Nonphononic vibrations originating from disordered structures have garnered significant attention as a fundamental feature of glasses that distinguishes them from crystals. Recently, we discovered that one-dimensional (1D) stringlike vibrations without volume change are responsible for the boson peak in the reduced density of states of two-dimensional (2D) glasses [Y.-C. Hu and H. Tanaka, Nat. Phys. 18, 669 (2022)]. Here we investigate the vibrational properties of three-dimensional (3D) model glasses with isotropic repulsive and attractive interactions and find that the boson peak arises from stringlike quasilocalized transverse vibrations in these 3D systems. These results suggest that stringlike vibrations are the universal origin of the boson peak in both 2D and 3D model glasses, as long as the interaction is isotropic. Furthermore, we confirm that the characteristic frequency of the quasilocalized transverse vibrations, i.e., the boson peak frequency, coincides with the Ioffe-Regel limit of transverse phonons. These results imply the boson peak originates from the frequency-resonant scattering of transverse phonons by quasilocalized vibrations rather than phonon scattering due to elastic inhomogeneity. Our findings provide insights into the origin of low-temperature glass anomalies and inspire further research.

Ce 3+:Lu 3Al 5O 12–Al 2O 3 optical nanoceramic scintillators elaborated via a low-temperature glass crystallization route

Transparent Ce:lutetium aluminum garnet (Ce:Lu₃Al₅O₁₂, Ce:LuAG) ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number (<i>Z</i>_eff). However, the current Ce:LuAG ceramics exhibit a light yield much lower than the expected theoretical value due to the inevitable presence of Lu_Al antisite defects at high sintering temperatures. This work demonstrates a low-temperature (1100 ℃) synthetic strategy for elaborating transparent LuAG–Al₂O₃ nanoceramics through the crystallization of 72 mol% Al₂O₃–28 mol% Lu₂O₃ (ALu28) bulk glass. The biphasic nanostructure composed of LuAG and Al₂O₃ nanocrystals makes up the whole ceramic materials. Most of Al₂O₃ is distributed among LuAG grains, and the rest is present inside the LuAG grains. Fully dense biphasic LuAG–Al₂O₃ nanoceramics are highly transparent from the visible region to mid-infrared (MIR) region, and particularly the transmittance reaches 82% at 780 nm. Moreover, Lu_Al antisite defect-related centers are completely undetectable in X-ray excited luminescence (XEL) spectra of Ce:LuAG–Al₂O₃ nanoceramics with 0.3–1.0 at% Ce. The light yield of 0.3 at% Ce:LuAG–Al₂O₃ nanoceramics is estimated to be 20,000 ph/MeV with short 1 μs shaping time, which is far superior to that of commercial Bi₄Ge₃O₁₂ (BGO) single crystals. These results show that a low-temperature glass crystallization route provides an alternative approach for eliminating the antisite defects in LuAG-based ceramics, and is promising to produce garnet-based ceramic materials with excellent properties, thereby meeting the demands of advanced scintillation applications.

Preparation and relationship between structure and properties of PTMEG based polyurethane acrylate UV cured films

A series of polyurethane acrylate UV curing films (FPUA) were designed and prepared from three different hard segment structure, hard segment content and NCO/OH molar ratio via prepolymer process from polytetramethylene ether glycol(PTMEG), diisocyanate and polycaprolactone modified acrylate (FM1D). And the influence of structural parameters on the cured films’ mechanical properties was studied; Besides, its thermal properties was characterized by Dynamic Thermomechanical Analysis (DMA) and Thermo Gravimetric Analyzer (TGA). Among these three hard segment structures, hexamethylene diisocyanate (HMDI) -based cured films have the best mechanical properties. The modulus and tensile strength of the cured films increases along with the increase of hard segment content, whereas the elongation at break of the cured films decreases since the rising of the NCO/OH molar ratio. Indeed, with hard segment content at 48.6% and NCO/OH molar ratio at 1.06, the UV cured films (exhibits the best performance)with tensile strength up to 50.5 MPa, and break elongation upto238%. DMA and TGA data showed that the low-temperature glass transition temperature of UV-cured films is around −50 °C, and the fastest thermal degradation temperature is 355 °C, showing good resistance to high and low temperatures.

Study on the Effect of Ultraviolet Absorber UV-531 on the Performance of SBS-Modified Asphalt.

Asphalt pavements at high altitudes are susceptible to aging and disease under prolonged action of UV light. To improve their anti-ultraviolet aging performance, UV-531/SBS-modified asphalts with UV-531 dopings of 0.4%, 0.7%, and 1.0% were prepared by the high-speed shear method, and the effect of UV-531 on the conventional performance of SBS-modified asphalt before aging was studied by needle penetration, softening point and 5 °C ductility tests. The high- and low-temperature rheological properties of UV-531/SBS-modified asphalt before and after aging were also analyzed by high temperature dynamic shear rheology test and low-temperature glass transition temperature test. Finally, the effect of UV-531 on the anti-aging performance of SBS-modified asphalt was evaluated by three methods, including rutting factor ratio, viscosity aging index, and infrared spectroscopy. The results show that with the increase of UV-531 doping, the needle penetration and 5 °C ductility show an increasing trend, but the effect on the softening point is small. The high temperature stability of SBS-modified asphalt is not much affected by the addition of UV-531, and the low-temperature stability is improved, and when 0.7% UV absorber is added, SBS-modified asphalt shows better low-temperature performance. The results of all three evaluation methods show that the addition of UV-531 significantly improved the anti-UV aging performance of SBS-modified asphalt, with the amount of 0.7% providing the asphalt with the best anti-UV aging performance. The results of the study can provide an important reference for improving the anti-ultraviolet aging performance of SBS-modified asphalt.

Sound attenuation in two-dimensional glasses at finite temperatures.

The thermal conductivity of glasses exhibits an unusual temperature dependence compared to their crystalline counterparts. Sound attenuation due to disorder in glasses was proposed to be important in rationalizing this special behavior. Simulation studies suggest that in the harmonic approximation, the sound attenuation follows Rayleigh scattering scaling at small wave vector in both two-dimensional (2D) and 3D glasses. The influence of the anharmonicity on sound attenuation has very recently been investigated numerically, but only in 3D glasses. Hence, it remains unknown in simulations how sound attenuation changes with the wave vector in 2D glasses when the anharmonicity comes into play. Here, we address this issue by performing computer simulations in low-temperature 2D glasses over a large range of glass stabilities. We find that the way the anharmonicity affects sound attenuation in 2D glasses is the same as that in 3D, thus revealing that numerically the influence of the anharmonicity on sound attenuation does not rely on the spatial dimension.