Design Of Materials Research Articles

Predicting the solid solution structure preference of multi-component alloys

High-entropy alloys (HEAs) provide limitless opportunities to enhance material performance while predicting the thermodynamic properties and the structures rapidly within HEAs remain challenging. Herein, a new method (M2FEn) for rapidly predicting the formation enthalpies is provided. In contrast to Miedema’s semi-empirical methodology, which solely calculates the mixing enthalpy, the M2FEn is capable of calculating the formation enthalpies of various solid solution structures, and by ordering these enthalpies, one can determine the preferred solid-solution structure for the single-phase alloy. The predicted structures using M2FEn are in line with first-principles calculations. The effectiveness of different extrapolation models for formation enthalpy has been assessed. The M2FEn with the Ouyang extrapolation model and the regular solution model have achieved a prediction accuracy of 95.8% and 95.4%, respectively for single-phase HEAs that were experimentally prepared. 28 common HEA elements were selected as the chemical space, and the formation enthalpies of all binary, ternary, quaternary, quinary and senary alloys, a total of 499149 various alloys were calculated by M2FEn. It is found that the BCC structure ratio increases with the increase of the principal element of the alloy. The M2FEn should potentially accelerate the development of novel, high-performance HEAs, enabling more efficient and cost-effective materials design processes.

Microstructural evolution and strengthening mechanism of TC4/ZTA composites fabricated by laser-directed energy deposition

In this study, zirconia-toughened alumina (ZTA) ceramics were prepared and used to fabricate crack-free, high-performance titanium alloy (TC4)/ZTA ceramic composites with a gradient material design through laser-directed energy deposition. The ZTA content gradients ranged from 0wt.% (0ZTA layer) to 20wt.% (20ZTA layer). During laser deposition, Ti reacted with Al2O3 in the ZTA ceramics to form TiAl2O5. Under rapid cooling in the non-preheated sample, the TiAl2O5 and ZrO2 in the 20ZTA layer underwent a phase transformation, resulting in the formation of TiAl2O5, Al2O3, and t-ZrO2. The cooling rate was lower in the preheated sample, which promoted the reaction between Ti and ZrO2, producing Ti2O. The stability of the β-Ti crystal structure was significantly affected by the presence of Al and Zr in the ZTA. First-principles calculations revealed that preheating caused a larger proportion of Al2O3 to melt, primarily destabilizing the β-phase through the action of Al. The reduction in the cooling rate also promoted the β → α phase transformation; making the α-phase dominant in the 20ZTA layer of the preheated sample. In the preheated sample, the hardness of the 20ZTA layer was 1.95 times greater than that of the 0ZTA layer, and the wear volume was reduced by 91.42%. The strengthening mechanisms in the 20ZTA layer, in descending order, were solid solution strengthening, dislocation strengthening, load transfer, and grain refinement.

Antioxidative implant coating with anti-infection and osteogenesis time-dependent bifunction for synergistic promotion of osteointegration

Infection and poor osteogenesis are two major causes of implant failure. Surface modification strategy provides solutions to the above problems. However, the functional requirements at different biological stages during infectious bone repair and the oxidative stimulation caused by reactive oxygen species (ROS) in an inflammatory environment pose challenges to the existing approaches. Layer-by-layer (LbL) self-assembly realizes layer by layer superposition and time-dependent acting of different bioactive components, but is demanding to functional groups. Tannic acid (TA) owns abundant phenolic hydroxyl groups, endowing various firm chemical bindings and excellent antioxidant property. To this end, we developed a time-dependent and antioxidant multifunctional coating via TA mediated LbL self-assembly. This layer exhibited higher ROS removal capacity and stronger binding ability. Furthermore, it showed rapid and excellent antibacterial ability of over 85 % against Staphylococcus aureus and Escherichia coli at 24 h, which additionally promotes osteogenic differentiation in vitro in long term. Moreover, the coating exhibited outstanding antibacterial and bone regeneration performance in vivo as well. Thus, this study is expected to provide an antioxidant and time-dependent multifunctional platform for surface modification engineering of dental and orthopedic implantation, as well as other potential biological material designs.

Enhanced buoyancy and propulsion in 3D printed swimming micro-robots based on a hydrophobic nano-fibrillated cellulose aerogel and porous lead-free piezoelectric ceramics

This paper provides the first demonstration of additively manufactured swimming micro-robots which combine a hydrophobic nanofibrillated cellulose aerogel, to provide long-term buoyancy, with a low acoustic impedance porous piezoelectric ceramic for improved propulsion. The hydrophobic nanocellulose aerogel is shown to exhibit a high and stable contact angle that was maintained for extended periods of time, which facilitates long-term and stable buoyancy of the micro-robot. To quantify the benefits of introducing porosity into the active piezoelectric element, a new analysis model was developed to inform material design and maximize the acoustic propulsion force. Detailed characterisation and modelling of the swimming robots demonstrated that a swimming robot based on a lead-free porous Ba0.85Ca0.15Zr0.1Ti0.9O3 (BCZT) ceramic exhibited a higher acoustic radiation propulsion force and a faster swimming speed compared to a robot fabricated using a dense ceramic element. These benefits were associated with the lower elastic modulus, density and acoustic impedance of the porous piezoelectric material. The lower dielectric constant, reduced device capacitance, and lower resonant frequency of the porous piezoelectric element also significantly reduced the driving current and power requirements of the robot. This work therefore provides new insights on the impact of hydrophobic and acoustically matched piezoelectric materials on the performance of swimming micro-robots, and successfully demonstrates the use of porosity to improve acoustic impedance matching of resonant piezoelectric devices, such as micro-robots and ultrasonic transducers.

Constitutive model and microstructure evolution of thermal deformation behavior of in situ TiB2p/Al-Zn-Mg-Cu composites with high Zn content

The deformation behavior of in situ TiB2 particle reinforced Al-Zn-Mg-Cu matrix composites with high Zn content was investigated through thermal compression tests. A comparative analysis of several constitutive models was performed, including the phenomenological modified Johnson-Cook (JC) and strain-compensated Arrhenius-type models, as well as the physically based modified and optimized Zerilli-Armstrong (ZA) models. In contrast to other materials, it is found that the accuracy of the modified JC and ZA models is significantly affected by the reference strain rate. When this was factored in, the optimized ZA model demonstrated superior accuracy, with a correlation coefficient (R) of 0.9986 and an average absolute relative error (AARE) of 2.15%, while requiring the fewest calculation efforts amongst all of the models attempted. The mechanisms of the microstructural evolution in the composites after thermal deformation were also investigated. This work advances the understanding of TiB2p/Al-Zn-Mg-Cu composites and introduces an improved modeling framework, which is expected to benefit future material design and performance.

Role of cerium modification on LDHs applied in three-dimensional electrochemical reactor for N-nitrosopyrrolidine disinfection by- products abatement in water

A three-dimensional electrochemical reactor (3DER) with Ce-modified CoFe-LDHs as particle electrodes is assembled and used to efficiently degrade N-Nitrosopyrrolidine (NPYRs) in disinfected water. The construction of hierarchical structure and oxygen vacancies accelerates the electron transfer rate, provides a suitable working potential range and reduces electrochemical resistance, which leads to improved removal efficiency. The optimised particle electrodes (Co2Fe0.84Ce0.16-LDHs@AC) achieved NPYR degradation of 81.5 % after 120 min of continuous treatment with low energy consumption of 2.4 kWh mg–1 NPYR (current density of 5 mA cm−2, flow rate of 3 mL min−1, electrolyte concentration of 0.21 mol L−1, and a pollutant concentration of 10 mg L−1). Based on GC-MS, LC-MS analysis and quenching experiments, the degradation pathway of NPYR is proposed, while reactive oxygen species (ROS) during the degradation process include •OH, O2•− and 1O2. The modification of Ce in LDHs has a significant role in enhancing degradation efficiency by accelerating the formation of ROS, which provides an efficient solution to the material design used in the 3DER system for boosting pollution degradation during water treatment.

An advanced ceramifical organic-inorganic hybrid polysiloxane coating with superior moisture-resistant property

A ceramifiable organic-inorganic hybrid polysiloxane, prepared via a straightforward solution blending method, was successfully coated on the surface of silicon dioxide ceramic via a scrapping method. A uniform and dense lithium aluminum borosilicon (LABS) vitrified layer in situ formed on the surface of silicon dioxide ceramics was successfully prepared through liquid phase filling method to fulfill the moisture resistance requirements under high temperature cycle conditions. Effects of aluminum content on the microstructure change process and moisture resistance properties of the ceramifiable organic-inorganic hybrid polysiloxane have been systematically researched. With the increase of aluminum content, the ceramic yield of the hybrid polysiloxane and the heat loss capacity of LABS glass-ceramics increase. The crack-free and high temperature fluid vitrified layer endows the LABS glass-ceramic with excellent thermal shock resistance cycle ability, self-healing ability and moisture resistance. Results showed that the LABS vitrified coating with an aluminum-boron ratio of 1:2 presents the most appealing thermal shock cycle resistance and crack self-healing ability after 20 thermal cycles, as well as a water absorption rate of 0.3814%. By refining the application of modified polysiloxane moisture-resistant coatings in high-temperature circulation environments, this work shed lights on the importance of in situ growth LABS vitrified coating in accelerating surface reconstruction and improving moisture resistance, incenting additional innovative breakthroughs in the LAS-based glass-ceramic materials design and fabrication within the aviation field.

Recent advances of organic long persistent luminescence: Design strategy and internal mechanism

AbstractOrganic afterglow materials have drawn increasing attention for their great potential in practical applications. Until now, most of them just show the lifetimes in milliseconds or seconds, while the realization of long persistent luminescence (LPL) lasting for minutes or even hours is difficult. In 2017, Adachi and Kabe successfully realize the LPL with a duration longer than 1 hour in a purely organic system, which can be even comparable to some excellent inorganic materials. However, partially for the unclear structure‐property relationship, organic LPL materials are still rather scarce, especially for the stable ones in air or aqueous solution. In this review, we present the recent progress in organic LPL, mainly focusing on the material design strategy and internal mechanism. It is anticipated that the deep understanding can be beneficial for the further development of organic LPL materials with good stability in air and even aqueous phase.

The reactivity of α-tricalcium phosphate powders is affected by minute amounts of β-calcium pyrophosphate and by the synthesis temperature

α-tricalcium phosphate (α-TCP) is the most widespread raw material for hydraulic calcium phosphate cements (CPCs). CPCs are widely used in bone repair due to their injectability, setting ability, and osteoconductivity. This study investigated the reactivity of α-TCP powders, focusing on the impact of minor phase impurities, β-calcium pyrophosphate and hydroxyapatite, and the synthesis temperature. The α-TCP powders were synthesized via a solid-state reaction of calcium carbonate and anhydrous dicalcium phosphate, with varying Ca/P molar ratios (1.4850-1.5075) and synthesis temperatures (1175°C-1350°C). Powders produced with a Ca/P molar ratio below 1.50 and synthesized at a temperature above the melting point of β-CPP (1296°C) had a broader size distribution and a two to fourfold lower hydraulic reactivity. Conversely, a higher Ca/P molar ratio improved reactivity. The study underscores the importance of precise control over synthesis parameters to enhance the performance of α-TCP-based CPCs, offering insights for optimizing material design in biomedical applications.

Thermal and Frequency Response Analysis on Friction Stir Welding Tool with Different Materials by Using FEA Method

Friction stir welding (FSW) is a solid-state joining technique that joins two facing workpieces without melting the workpiece material. It makes use of a deceased item. The region surrounding the FSW tool softens due to heat produced by friction between the revolving tool and the workpiece material. We are now working on specialised applications (lap and butt welding) while concentrating on test sorts. In addition to being faster than the state of the art, both provide lap welds that are 190% of the plate thickness, improve weld honesty, and lessen upper plate decline. Friction stir welding, or FSW for short, is a popular solid state joining method for soft materials like aluminium alloys. For stronger alloys like steel and titanium alloys, the FSW process's economic sustainability hinges on the creation of long-lasting, moderately cost equipment that reliably yields welds with outstanding structural integrity. The performance of the tool, weld quality, and cost are all impacted by material design and choice. This research reviews and critically examines many key FSW tool components, including process economics, geometry and load bearing capacity, frequency response analysis, tool degradation mechanisms, and tool material selection. The Finite Element Method (FEM) approach is used to characterise the process and provide a more comprehensive knowledge of the thermal effects and thermal inaccuracies on the tool materials.

Storage Mechanism and Structural Design of High-Performance Renewable Hydrogen Storage Materials Derived from Biomass-Based Porous Carbon: A Mini-Review

Storage Mechanism and Structural Design of High-Performance Renewable Hydrogen Storage Materials Derived from Biomass-Based Porous Carbon: A Mini-Review

Synthesis and characterization of new perylenediimide derivatives: Promising low-cost electron transport materials for perovskite solar cells

In organic-inorganic perovskite solar cells (PSCs), the electron transport layer (ETL) plays a crucial role providing efficient electron extraction and transport required for achieving high device performance. Compared to traditional fullerene-based electron-transport materials (ETMs), non-fullerene small molecules have attracted much attention due to their tunable optoelectronic properties, lower cost, and much higher stability. In this work, we synthesized and characterized four perylenediimide (PDI) derivatives and investigated their optoelectronic properties in the context of application as ETMs for PSCs. To establish the compatibility of PDI films with perovskite absorber material, the surface properties of Cs0.12FA0.88PbI3/PDI bilayer stacks were studied using contact angle and infrared scattering scanning near-field microscopy methods. A study of the photochemical stability of these bilayer stacks showed that coating the perovskite film with a layer of PDI improves its tolerance with respect to light. Utilizing these molecules as ETMs in the inverted p-i-n PSCs delivered light power conversion efficiencies ranging from 11.1 % to 15.4 %, thus indicating the considerable effect of the PDI derivative molecular structure on the photovoltaic properties. Further development of this research direction may lead to the rational design of advanced PDI-based electron transport materials for efficient and stable PSCs.

Unraveling how hydrogen-bonding networks affect the capture of amphetamine-type stimulants by polymerized deep eutectic solvent modified magnetic biochar: Coupling quantum chemical calculations with experiment

The abuse of amphetamine-type stimulants (ATSs) has caused irreversible harm to public safety and ecosystems. A novel polymerized deep eutectic solvent modified magnetic pomelo peel biochar (PMBC) was prepared, and the differences in adsorption of four abused amphetamine-type stimulants (ATSs: AMP, MAMP, MDA and MDMA) were due to varying hydrogen bonds quantities and strengths. PMBC showed excellent chemical reactivity to MDMA, with a maximum adsorption capacity of 926.13 μg g−1, which was 3.25, 2.52 and 1.15 times higher than that of AMP, MAMP and MDA, respectively. Modern spectral analysis showed that there were a series of active centers (-COOH, -NH2 and -OH) on the PMBC, which could form hydrogen bond networks with the nitrogen and oxygen functional groups of ATSs. In various chemical environments: pH level (4–11), inorganic ion and organic matter (humic acid), PMBC maintained high activity towards four ATSs. Additionally, the quantum chemical calculations revealed that the methylenedioxy bridge of ATSs can increase the active sites, and the -NH- and -NH2 groups had different hydrogen bond formation capabilities, which together resulted in the adsorption order of PMBC on the four ATSs: MDMA > MDA > MAMP > AMP. Moreover, the hydrogen-bonding binding energies of several common hydrogen-bonding types were compared, including O-H····O, N-H····O/O-H····N and N-H···N. This study laid an empirical and theoretical foundation for the efficient capture of ATSs in water and contributed to the innovative design of materials.

Additive manufacturing of polymer composite millimeter‐wave components: Recent progress, novel applications, and challenges

AbstractWith the advent of 5G/6G for radar and space communication systems, various millimeter‐wave (MMW) components are rapidly innovated for multi‐functional, higher integrated and miniaturized solutions across diverse industries and applications. Polymer composites‐based additive manufacturing (AM), an advanced manufacturing technique, can manufacture MMW components with high fabrication resolution, intricate structural design, adjustable dielectric properties, and functionally gradient distribution characteristics. This paper outlines the state‐of‐the‐art polymer composite MMW components, their design, and manufacturing techniques. An integrated “material‐structure‐manufacturing‐performance” design conceptual framework of polymer composite MMW components is discussed in terms of material design, structure design, and process design. Moreover, multi‐functional polymer composite MMW structures focus on electromagnetic wave absorption and electromagnetic interference (EMI) shielding functions. Moreover, novel applications of MMW polymer composite components enabled by AM on radar/sensing, communication, enclosure, and miscellaneous applications are discussed. Furthermore, future perspectives and current challenges are identified to provide new insights into multi‐functional 3D‐printed MMW products, exploring new possibilities for next‐generation advanced MMW technology.Highlights The 3D‐printed MMW components and additive manufacturing are reviewed. The integrated “material‐structure‐manufacturing‐performance” concept is introduced. 3D‐printed MMW components are discussed on radar, enclosure, and miscellaneous applications. Future perspectives and challenges of 3D‐printed MMW components are addressed.

Micro-mechanical properties of Song Dynasty tilestones based on nanoindentation tests and homogenization approach

Song Dynasty tilestones are one type of ancient Chinese building materials. Studying their mechanical properties is of great significance for the design and development of restoration materials. It is a challenge to sample and perform traditional tests (ϕ50mm × 100mm) for the tilestone cultural relics. In this work, a combination of nanoindentation techniques and the homogenization calculation method based on the Mori–Tanaka model were used to determine the mechanical parameters of Song Dynasty tilestones. The study process involved several steps: (1) Using X-ray diffraction and scanning electron microscopy to examine the surface morphology and mineral composition of the tilestones. (2) Determining the mechanical parameters (i.e., the elastic modulus, hardness and fracture toughness) through nanoindentation tests. (3) Upgrading mechanical parameters from micro to meso-scale using the Mori–Tanaka model and comparing these with uniaxial compression test results. The result shows that the red tilestones and green tilestone are mainly composed of quartz, feldspar and mica. The average elastic modulus of the red tilestones and the green tilestones are 29.47 GPa and 30.21 GPa, respectively. Compared with the parameter result obtained by upscaling, the deviation rates of the red tilestones and green tilestones are 10.3% and 9.6%, respectively, which proves that the test method is reliable. The nanoindentation test and homogenization approach in this work provide the robust theoretical and practical basis for evaluating the mechanical strength of Song Dynasty tilestones.

Interplay of Na Substitution in Magnetic Interaction and Photocatalytic Properties of Ca1-xNaxTi0.5Ta0.5O3 Perovskite Nanoparticles.

This research paper delves into the enhancement of wastewater treatment through the design and synthesis of advanced photocatalytic materials, focusing on the effects of sodium (Na) substitution in Ca1-xNaxTa0.5Ti0.5O3 perovskites. By employing various analytical techniques such as X-ray diffraction, Field Emission Scanning Electron Microscopy, Transmission Electron Microscopy and UV-vis spectroscopy, the study examines the transition of these perovskites from tetragonal to orthorhombic structures and observes a reduction in Ca content with Na substitution, which also favors the cubic phase formation and inhibits secondary phases. Significantly, magnetic property analysis uncovers an unexpected ferromagnetic ordering in these perovskites, including compositions traditionally viewed as non-magnetic. The photocatalytic tests reveal a significant improvement in degrading Rhodamine B dye under visible light, particularly in samples with higher Na levels, attributed to enhanced light absorption and efficient electron processes. The study highlights the optimal Na substitution level for peak photocatalytic performance, offering valuable insights into the complex interplay between structural, magnetic, and photocatalytic properties of these perovskites, and their potential in various applications, thereby contributing to the advancement of wastewater treatment technologies.

Energetic Methylene-Bridged Furoxan-Triazole/Tetrazole Hybrids.

Design and synthesis of new energetic materials retains its urgency in chemistry and materials science. Herein, rational construction and regioselective synthesis of a series of energetic compounds comprising of a methylene-bridged combination of 1,2,5-oxadiazole and nitrogen-rich azoles (1,2,4-triazole and tetrazole) enriched with additional explosophoric functionalities (nitro and azo moieties) is presented. All target materials were thoroughly characterized using IR and multinuclear NMR (1H,13C,14N,15N) NMR spectroscopy, high-resolution mass spectrometry, X-ray diffraction,and differential scanning calorimetry. All synthesized energetic substances showed good thermal stability (up to 239oC) and low mechanical sensitivity, while their performance reached or exceeded the level of TNT.

Evolution of Confinement Stress in Axially Loaded Concrete-Filled Steel Tube Stub Columns: Study on Enhancing Urban Building Efficiency

In the context of green building and sustainable urban development, understanding the mechanical behavior of structural components like concrete-filled steel tube (CFST) columns is crucial due to their improved load-bearing capacity, energy efficiency, and optimized material usage, which enhance structural resilience and sustainability. This research addresses the complex development of confining stress and its impact on the concrete core (CC) behavior within these columns, which are essential for urban infrastructure. Through extensive numerical studies, this study proposes a model to estimate the confining stress in axially loaded CFST short columns. Study findings reveal that the confinement effectiveness is influenced by variables such as compressive strength (CS) of the concrete, cross-sectional shape, and depth-to-wall thickness percentage. Additionally, the confinement is also significantly affected by the yield strain of steel εy/εc to the peak strain of unconfined concrete εc. A three-dimensional finite element model (FEM) was built for the simulation of the columns’ nonlinear behavior and was rigorously validated against experimental data. This model aids in the design and implementation of more efficient and resilient urban structures, supporting the principles of sustainable construction. The study underscores the importance of structural integrity in sustainable urban development and provides valuable insights for improving the design of green building materials.

Protein-driven interaction enhanced electrochemiluminescence biosensor of hydrogen-bonded biohybrid organic frameworks for sensitive immunoassay of disease markers

The oriented design of reticular materials as emitters can significantly enhance the sensitivity of electrochemiluminescence (ECL) sensing analysis for disease markers. However, due to the structural fragility of hydrogen bonds, relational research on hydrogen-bonded organic frameworks (HOFs) has not been thoroughly conducted. Additionally, the modulation of luminescence behavior through HOFs has been rarely reported. In view of this, hydrogen-bonded biohybrid organic frameworks (HBOFs) were synthesized and recruited for ECL immunoassay applications. HBOFs was easily prepared using 6,6′,6″,6‴-(pyrene-1,3,6,8-tetrayl)tetrakis(2-naphthoic acid) as linkers via bovine serum albumin (BSA) activated hydrogen-bonded cross-linking. The material exhibited good fluorescence emission characteristics. And the highly ordered topological structure and molecular motion limitation mediated by BSA overcome aggregation-caused quenching and generate strong aggregation induced emission, expressing hydrogen-bond interaction enhanced ECL (HIE-ECL) activity with the participation of tri-n-propylamine. Furthermore, a sandwich immunosensor was constructed employing cobalt-based metal-phenolic network (CMPN) coated ferrocene nanoparticles (FNPs) as quenchers (CMPN@FNPs). Signal closure can be achieved by annihilating the excited state through electron transfer from both CMPN and FNPs. Using a universal disease marker, carcinoembryonic antigen, as the analysis model, the signal-off sensor obtained a detection limit of 0.47 pg/mL within the detection range of 1 pg/mL - 50 ng/mL. The synthesis and application of highly stable HBOFs triggered by proteins provide a reference for the development of new reticular ECL signal labels, and electron transfer model provides flexible solutions for more sensitive sensing analysis.

Putting error bars on density functional theory

Predicting the error in density functional theory (DFT) calculations due to the choice of exchange–correlation (XC) functional is crucial to the success of DFT, but currently, there are limited options to estimate this a priori. This is particularly important for high-throughput screening of new materials. In this work, the structure and elastic properties of binary and ternary oxides are computed using four XC functionals: LDA, PBE-GGA, PBEsol, and vdW-DF with C09 exchange. To analyze the systemic errors inherent to each XC functional, we employed materials informatics methods to predict the expected errors. The predicted errors were also used to better the DFT-predicted lattice parameters. Our results emphasize the link between the computed errors and the electron density and hybridization errors of a functional. In essence, these results provide “error bars” for choosing a functional for the creation of high-accuracy, high-throughput datasets as well as avenues for the development of XC functionals with enhanced performance, thereby enabling the accelerated discovery and design of new materials.