Synthesis Of Materials Research Articles

Predicting emergence of crystals from amorphous precursors with deep learning potentials.

Crystallization of amorphous precursors into metastable crystals plays a fundamental role in the formation of new matter, from geological to biological processes in nature to the synthesis and development of new materials in the laboratory. Reliably predicting the outcome of such a process would enable new research directions in these areas, but has remained beyond the reach of molecular modeling or ab initio methods. Here we show that candidates for the crystallization products of amorphous precursors can be predicted in many inorganic systems by sampling the local structural motifs at the atomistic level using universal deep learning interatomic potentials. We show that this approach identifies, with high accuracy, the most likely crystal structures of the polymorphs that initially nucleate from amorphous precursors, across a diverse set of material systems, including polymorphic oxides, nitrides, carbides, fluorides, chlorides, chalcogenides and metal alloys.

Composite material from polylactic acid and modified fire flax: synthesis and properties

Abstract The paper presents data on the synthesis of a composite material based on polylactic acid and fire flax powder. To improve adhesion between the polymer matrix and the plant filler, the fire flax powder was modified (acylated) with acetic anhydride. The IR Fourier spectroscopy method established the acylation reaction of fire flax powder. After modification with acetic anhydride, an increase in the intensity of the following peaks is observed in the IR Fourier spectrum: at 1747 cm-1, at 1374 cm-1 and at 1234 cm-1. Composites based on polylactic acid were manufactured, which contained the modified filler in concentrations of 30%, 40% and 50% by weight. Physicomechanical, electron microscopic and thermal studies of the developed polymer composites are presented. The tensile strength of the studied composites was determined using standard methods according to ISO 527-2:2012. The composite containing 50 wt. % modified fire flax powder has the following characteristics: tensile strength – 6.53 MPa, relative elongation - 13.89%, density - 1.247 g/cm3, maximum permissible operating temperature (sample weight loss up to 5 wt. %) - 254 ° C. This study promotes the development of biodegradable materials by offering polylactide-based composites with the addition of fire flax as an alternative to non-degradable synthetic fillers. The use of agricultural waste not only reduces the cost of production, but also solves the problem of biomass utilization, which opens up prospects for the creation of environmentally friendly composites in various industries. The research methodology also makes it possible to modify natural components, expanding their use and potentially replacing traditional plastics.

The Synthesis, Characteristics, and Application of Hierarchical Porous Materials in Carbon Dioxide Reduction Reactions

The reduction of carbon dioxide to valuable chemical products could favor the establishment of a sustainable carbon cycle, which has attracted much attention in recent years. Developing efficient catalysts plays a vital role in the carbon dioxide reduction reaction (CO2RR) process, but with great challenges in achieving a uniform distribution of catalytic active sites and rapid mass transfer properties. Hierarchical porous materials with a porous hierarchy show great promise for application in CO2RRs owing to the high specific surface area and superior porous connection. Plenty of breakthroughs in recent CO2RR studies have been recently achieved regarding hierarchical porous materials, indicating that a summary of hierarchical porous materials for carbon dioxide reduction reactions is highly desired and significant. In this paper, we summarize the recent breakthroughs of hierarchical porous materials in CO2RRs, including classical synthesis methods, advanced characterization technologies, and novel CO2RR strategies. Moreover, by highlighting several significant works, the advantages of hierarchical porous materials for CO2RRs are analyzed and revealed. Additionally, a perspective on hierarchical porous materials for CO2RRs (e.g., challenges, potential catalysts, promising strategies, etc.) for future study is also presented. It can be anticipated that this comprehensive review will provide valuable insights for further developing efficient alternative hierarchical porous catalysts for CO2 reduction reactions.

The Changing Landscape of Materials Discovery.

In this perspective, we will discuss the impact of some of the most recent advancements in materials discovery, particularly focusing on the role of robotics, artificial intelligence, and self-driving laboratories, as well as their implications for the Swiss research landscape. While it seems timely to aim for broad, revolutionary breakthroughs in this field, we argue that more incremental steps - such as, for example, fully automatic grinding of solid powders or fully automated Rietveld refinements - may have a more significant impact on materials discovery, at least in the short run. In the center of these considerations is how small, interdisciplinary groups can drive significant progress by contributing targeted innovations, such as e.g.robotic sample preparation or computational predictions. Additionally, given the large investments that are necessary for future infrastructures in materials discovery, we discuss the potential case for the establishment - in the long run - of a national infrastructure, a Swiss Materials Discovery Lab, to support automated material synthesis and advanced characterization, ultimately accelerating innovation in both academic and industrial settings.

Tailoring Ga‐Doped ZnO Thin Film Properties for Enhanced Optoelectric Device Performance: Argon Flow Rate Modulation and Dynamic Sputtering Geometry Analysis

The impact of dynamic sputtering geometry on the properties of ZnO: Ga (GZO) thin film nanomaterials is investigated by systematically varying Ar flow rates and substrate positions during the film growth. The structural, optical, and electrical characteristics of GZO layers, deposited from a ZnO: Ga (5.7 wt%) ceramic‐type sputtering target, are comprehensively evaluated to reveal the relationship between the sputtering geometry and material properties. The obtained electrical properties, comparatively high carrier mobility 11.3 × 101 cm2 V−1 s−1 and the lowest resistivity 1.13 × 10−3 Ω‐cm, together with a moderately high optoelectric figure of merit with the films prepared using around 6 sccm Ar‐flow rate (corresponding to around 4.92 mTorr Ar partial pressure) reveal distinct correlations between the sputtering conditions and thin film properties, providing insights into the optimization of sputtering parameters for tailored material synthesis required for advanced and emerging applications. The GZO thin film (prepared with the optimal setting of 6 sccm Ar flow rate) exhibits remarkable optoelectronic capabilities as a transport layer in solar cells, reaching peak efficiencies of 26.34% for CIGS, 14.142% for CdTe, and 24.289% for Cs2AgBiBr6 perovskite in SCAPS‐1D simulated models. This study advances sputtering techniques for precise engineering of functional nanomaterials with enhanced performance and versatility, contributing to material synthesis optimization for emerging applications.

The Influence of the Solid Phase on the Properties of Foam Concrete

An overview of literary sources related to the formation and development of the technology of aerated concrete is given. It is shown and systematized in which directions scientific research aimed at improving their functional properties was conducted. It is noted that almost all researchers associate the dependence of the properties of porous concrete with the character of their porosity. The conducted analysis allowed the authors to hypothesize that the properties of aerated concrete are exclusively determined by the nature of the distribution of the solid phase, that is, by the nature of its structure. Determination of the influence of the solid phase and its nature on the properties of aerated concrete is devoted to experimental studies. They were conducted in two stages. At the first, when applying physical modeling, the effect of the total porosity and water consumption of the dry mixture on the change in the nature of the solid phase of the model was studied. Internal interfaces between structural elements are taken as characteristics of the solid phase - their total length and width. It is shown that the water consumption of the mixture has different effects on materials with a dense and porous structure. At the next stage of experimental research, the influence of the water consumption of the mortar mixture on its strength (strength of the matrix material) and the strength of foam concrete was studied. The initial rheological conditions of the formation of the structure were changed by changing the size and amount of filler, changing the amount of liquid and plasticizing additives. The results of the experiments confirmed that the initial rheological conditions have different effects on the materials of dense and porous structure. Under certain conditions, in materials with a porous structure (in foam concrete), an increase in the water-solid ratio leads to an increase in the strength of concrete. Which indicates that with such water consumption, more favorable conditions are created for the formation of a porous structure, which is reproduced on the character of the solid phase. The given results confirm the given hypothesis and can be used in the synthesis of new building materials, including with the use of artificial intelligence.

Influence of Copper and Tin Oxidation States on the Phase Evolution of Solution-Processed Ag-Alloyed CZTS Photovoltaic Absorbers

Kesterite-based semiconductors, particularly copper–zinc–tin–sulfide (CZTS), have garnered considerable attention as potential absorber layers in thin-film solar cells because of their abundance, nontoxicity, and cost-effectiveness. In this study, we explored the synthesis of Ag-alloyed CZTS (ACZTS) materials via the sol–gel method and deposited them on a transparent fluorine-doped tin oxide (FTO) back electrode. A key challenge is the selection and manipulation of metal–salt precursors, with a particular focus on the oxidation states of copper (Cu) and tin (Sn) ions. Two distinct protocols, varying the oxidation states of the Cu and Sn ions, were employed to synthesize the ACZTS materials. The transfer from the solution to the precursor film was analyzed, followed by annealing at different temperatures under a sulfur atmosphere to investigate the behavior and growth of these materials during the final stage of annealing. Our results show that the precursor transformation from solution to film is highly sensitive to the oxidation states of these metal ions, significantly influencing the chemical reactions during sol–gel synthesis and subsequent annealing. Furthermore, the formation pathway of the kesterite phase at elevated temperatures differs between the two protocols. Structural, morphological, and optical properties were characterized via X-ray diffraction (XRD), Raman spectroscopy, and scanning electron microscopy (SEM). Our findings highlight the critical role of the Cu and Sn oxidation states in the formation of high-quality kesterite materials. Additionally, we studied a novel approach for controlling the synthesis and phase evolution of kesterite materials via molecular inks, which could provide new opportunities for enhancing the efficiency of thin-film solar cells.

High-Efficiency Broad-Spectrum Antibacterial Activity of Chitosan/Zinc Ion/Polyoxometalate Composite Films for Water Treatment.

The development of multifunctional films with rapidly killing microorganisms and adsorbing residual antibiotics in wastewater remains a challenging endeavor. In this work, the chitosan/zinc ion/polyoxometalate (CS/Zn2+/POM) multifunctional films were prepared by the freeze-drying method using chitosan, ZnO, and POM. Notably, the CS/Zn2+/POM films exhibited excellent bactericidal properties against Gram-positive/negative bacterial strains including Staphylococcus aureus (S. aureus, 99.80%), Escherichia coli (E. coli, 99.82%), and drug-resistant E. coli bacterial strains (kanamycin-resistant E. coli, 87.76% and ampicillin-resistant E. coli, 99.71%). This may be due to the chelation of Zn2+ with CS disrupting the cell membrane and bringing POM into direct contact with bacteria, leading to bacterial death. In addition, the CS/Zn2+/POM films showed good adsorption performance to a tetracycline (TC) solution (adsorption rate 75.2%). Further studies showed that the main process of tetracycline removal by CS/Zn2+/POM films was controlled by a physical adsorption. This POM-based film material has an important potential for the synthesis of broad-spectrum antimicrobial materials for the removal of residual antibiotics from water pollutants such as tetracycline.

Application of Voronoi Polyhedra for Analysis of Electronic Dimensionality in Emissive Halide Materials.

The synthesis of new hybrid halide materials is attracting increasing research interest due to their potential optoelectronic applications. However, general design principles that explain and predict their properties are still limited. In this work, we attempted to reveal the role of intermolecular interactions on the optical properties in a series of hybrid halides with an (EtnNH4-n)2Sn1-xTexCl6 (n = 1-4) composition. DFT calculations showed that the dispersions of the bands involving the Te 5s orbital character gradually decrease as the size of the organic cation increases, indicating a reducing orbital overlap between neighboring TeCl62- complexes. We characterized the photoluminescence (PL) of the Sn/Te solid solutions in (EtnNH4-n)2Sn1-xTexCl6 (n = 1-4) phases to correlate the electronic and optical properties. The PL response shows no concentration quenching effects in the (Et4N)2Sn1-xTexCl6 series, which demonstrated electronically isolated TeCl62- complexes. However, the series with smaller organic cations (n = 1-3) and higher electronic dimensionality show concentration quenching effects, which decrease as a function of the Te 5s band dispersions in these compounds. Similar trends can be revealed using a simple semiquantitative electronic dimensionality analysis method by means of Voronoi polyhedra. Since this approach relies only on structural data, it enables rapid characterization of orbital overlap between metal halide complexes in hybrid materials without DFT calculations. The present results allow us to conclude that electronic dimensionality plays an essential role in the photophysical properties of hybrid halide compounds and can be used to fine-tune their properties.

Proofreading mechanism for colloidal self-assembly

Designing components that can robustly self-assemble into structures with biological complexity is a grand challenge for material science. Proofreading and error correction is required to improve assembly yield beyond equilibrium limits, using energy to avoid kinetic traps in the energy landscape. Here, we introduce an explicit two-staged proofreading scheme for patchy particle colloidal assemblies that substantially improves assembly yield and robustness. The first stage implements local rules whereby particles increase their binding strengths when they detect a local environment corresponding to a desired target. The second stage corrects remaining errors, adding a reverse pathway inspired by kinetic proofreading. The scheme shows significant yield improvements, eliminating kinetic traps, giving a much broader temperature range with high yield. Additionally, the scheme is robust against quenched disorder in the components. Our findings illuminate a pathway for advancing the programmable design of synthetic living materials, potentially fostering the synthesis of novel biological materials and functional behaviors. Published by the American Physical Society 2024

Miniaturize the Redox Flow Battery for Accelerated Materials Discovery and Development

Abstract Redox flow batteries are a promising technology for grid-scale energy storage. The aqueous organic redox flow battery is of particular interest for its potentially low material cost and sustainability. Developing novel organic active material for flow battery electrolytes typically entails molecular engineering toward desired properties, necessitating organic synthesis. In a research laboratory setting, the synthesis of specifically designed organic molecules featuring targeted functional groups is time and resources intensive. In the past, synthesizing materials required for battery testing has often required gram-scale production, presenting considerable constraints on the pace of novel organic material discovery. In this report, we introduce a miniaturized cell design that mandates only milligram-scale material synthesis while yielding testing outcomes equivalent or superior to those reported with other commercially available or homemade flow cells in the literature. The test results under various pH conditions validate the scale-down strategy to accelerate the flow battery material discovery and development using the newly designed mini cell. This approach offers researchers an efficient means to notably reduce the time and resource required to develop novel materials for flow batteries.

Self-driving AMADAP laboratory: Accelerating the discovery and optimization of emerging perovskite photovoltaics

AbstractThe development of new solar materials for emerging perovskite photovoltaics poses intricate multi-objective optimization challenges in a large high-dimensional composition and parameter space, with in some cases, millions of potential candidates to be explored. Solving it necessitates reproducible, user-independent laboratory work and intelligent preselection of innovative experimental methods. Materials Acceleration Platforms (MAPs) seamlessly combine robotic materials synthesis, characterization, and AI-driven data analysis, enabling the exploration of new materials. They revolutionize material development by replacing trial-and-error methods with precise, rapid experimentation and generating high-quality data for training machine learning (ML) algorithms. Device Acceleration Platforms (DAPs) focus on optimizing functional energy films and multilayer stacks. Unlike MAPs, DAPs concentrate on refining processing conditions for predetermined materials, crucial for disordered semiconductors. By fine-tuning processing parameters, DAPs significantly advance disordered semiconductor devices such as emerging photovoltaics. This article examines recent advancements in automated laboratories for perovskite material discovery and photovoltaics device optimization, showcasing in-house-developed MAPs and a DAP. These platforms cover the entire value chain, from materials to devices, addressing optimization challenges through robot-based high-throughput experimentation (HTE). Ultimately, a self-driven Autonomous Material and Device Acceleration Platforms (AMADAP) laboratory concept is proposed for autonomous functional solar material discovery using AI-guided combinational approaches. Graphical abstract

Compass-model physics on the hyperhoneycomb lattice in the extreme spin-orbit regime

The physics of spin-orbit entangled magnetic moments of 4d and 5d transition metal ions on a honeycomb lattice has been much explored in the search for unconventional magnetic orders or quantum spin liquids expected for compass spin models, where different bonds in the lattice favour different orientations for the magnetic moments. Realising such physics with rare-earth ions is a promising route to achieve exotic ground states in the extreme spin-orbit limit; however, this regime has remained experimentally largely unexplored due to major challenges in materials synthesis. Here we report the successful synthesis of powders and single crystals of β-Na2PrO3, with 4f1 Pr4+ jeff = 1/2 magnetic moments arranged on a hyperhoneycomb lattice with the same threefold coordination as the planar honeycomb. We find a strongly non-collinear magnetic order with highly dispersive gapped excitations that we argue arise from frustration between bond-dependent, anisotropic off-diagonal exchanges, a compass quantum spin model not explored experimentally so far. Our results show that rare-earth ions on threefold coordinated lattices offer a platform for the exploration of quantum compass spin models in the extreme spin-orbit regime, with qualitatively distinct physics from that of 4d and 5d Kitaev materials.

Terminal Effects of Fulleropyrrolidine Electron Transport Materials for Efficient Perovskite Solar Cells

AbstractFullerene (C60) and its derivatives are the most prevalent and efficient electron transport materials (ETMs) for state‐of‐the‐art perovskite solar cells (PSCs). Benefiting from the high performance, simple synthesis, and easy availability of raw materials, fulleropyrrolidine derivatives (FDs) are potential next‐generation ETM alternatives to currently used fullerene materials. However, the power conversion efficiency (PCE) of FDs still lags far behind that of methanofullerene derivatives such as [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM). Moreover, the underlying mechanism remains unclear. In this work, six FD ETMs are designed and synthesized, i.e., CN‐TPAX (X = H, Me, OMe, Cl, Br, I), for p‐i‐n PSCs, and obtained a champion PCE of over 25% for the CN‐TPACl ETM, outperforming all reported FDs until now. Subsequently, their performance is systematically characterized in terms of molecular characteristics, including single‐crystal structure, electronic properties, film formability/morphology, and electron dynamics, which helped reveal the terminal effects of FD ETMs on the molecular characteristics and photovoltaic performance of PSCs. This approach clarified the structure–performance relationships between the FDs and the resulting devices, highlighting the importance of the terminal design of fullerene ETMs for high‐performance PSCs.

Preparation and characterisation of novel foamed porous glass-ceramics on the basis of bioglass 45S5

This study determines the possibilities of synthesis of porous glass-ceramic materials based on Bioglass 45S5 using different methods obtained porous materials. In this work used foaming with sintering method for the set: bioglass 45S5 + glass cullet (CRT) + glass water (WG) and method sintering with forming-pore agents for the: bioglass + glass water (WG) + dried banana peels. The sets were melting and the next step sintering process. The resulting foams were examined and analysed for structural, microstructural, and physical properties. The research allowed for a quantitative and qualitative assessment of the foaming process generated by the presence of WG with the addition of CRT cullet and WG together with dried banana peel. It was found that WG with the addition of CRT cullet was a solution that offered the possibility of obtaining a large number of evenly distributed pores and higher total porosity compared the second set (WG + banana peel). Moreover, the use of CRT cullet and banana peel allowed the introduction of biogenic elements such as strontium, barium and potassium into the obtained materials, which have a positive effect on the stimulation of osteogenesis.

Symmetry and Asymmetry in Mutations and Memory Retention during the Evolutionary Growth of Carbon Nanotubes.

Symmetry is a motif featured in almost all areas of science, and understanding the mechanism of symmetry breaking is challenging. Similar to mutations that disrupt symmetry in evolution, defects in materials offer insight into symmetry breaking. Here, we investigate symmetry in intragenerational mutations and symmetry breaking in transgenerational mutations in the evolutionary growth system of carbon nanotubes (CNTs). Mutations caused by pentagon-heptagon (5-7) pairs in different conformations shorten the lifespans of single-walled carbon nanotubes (SWNTs) by acting as time markers during growth. Symmetric distributions are observed for intragenerational mutations from (n, m) to (n + i, m-i) (where i ∈ caslon Z) with different appearance orders of pentagon and heptagon. Such symmetry breaks occur in transgenerational mutations. Intragenerational mutations occur multiple times on a SWNT, oscillating regularly between i and - i until termination occurs. These types and effects are retained in the form of memory to encode SWNTs during subsequent growth, resulting in a length reduction after each mutation. Our results provide a profound understanding of symmetry breaking and memory retention and offer guidance for the controlled synthesis of materials.

Porous Materials for the Heterogeneously Catalyzed Synthesis of High Value-Added Products: Latest Trends and Future Prospects.

Heterogeneous catalysis currently stands as a foundational area in materials synthesis and applied chemistry. In this context, emphasizing the significance of heterogeneous catalysis in expediting chemical reactions and controlling the formation of desired products using porous materials represents an intriguing approach in the current technological landscape. This work delves into the synthesis and design of a variety of porous materials, encompassing microporous, mesoporous and macroporous materials (e. g. carbonaceous materials, metal oxides, MOFs, zeolites and functionalized analogues), alongside their properties and characteristics pivotal in heterogeneous catalysis. among others, and their subsequent modification, underscoring the significance of tailoring porous materials for specific catalytic applications.

Synthesis of high-entropy materials

Synthesis of high-entropy materials

Effect of high-temperature shear deformation on the synthesis of TiB<sub>2</sub>‒ZrO<sub>2</sub> composite material under conditions of free SHS compression

Ceramic materials based on TiB2 and stabilized ZrO2 were obtained by self-propagating high-temperature synthesis (SHS). The stabilization of the high-temperature phases of ZrO2 was carried out by introducing Y2O3 into the initial mixture. The effect of the Y2O3 content on the combustion characteristics of the studied materials, as well as on the phase composition of synthesis products in the range of Y2O3 concentrations from 0 to 6,2 wt. %, was studied. Gorenje. To study the effect of high-temperature shear deformation on the synthesis process by free SHS compression, compact plates with dimensions of 50×50×7 mm were obtained based on the studied compositions. It has been established that as a result of the synthesis of materials obtained under conditions of high-temperature shear deformation and without pressure application, the reaction products have different phase compositions. The resulting compact plates are composite materials consisting of a matrix based on stabilized ZrO2 with TiB2 particles distributed in it.

Viscoelastic ordering in microfluidic devices: current knowledge, open questions and challenges

Abstract Objects flowing in microfluidic devices can self-organise in ordered structures thanks to the hydrodynamic interactions mediated by either inertial or viscoelastic forces. Such structures have been found to be crucial to enhancing microfluidic applications such as single encapsulation, co-encapsulation, and material synthesis. However, while inertial ordering has been investigated in more detail, studies on viscoelastic ordering are much more limited. In this perspective, we report the recent advancements in viscoelastic ordering while also discussing the open questions and challenges related to this field. We also include a brief description of both experimental and numerical protocols that can be employed to investigate viscoelastic ordering.