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6,828 result(s) for "structural evolution"
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Phase and Structural Thermal Evolution of Bi–Si–O Catalysts Obtained via Laser Ablation
Laser methods are successfully used to prepare complex functional nanomaterials, especially for biomedicine, optoelectronics, and heterogeneous catalysis. In this paper, we present complex oxide and composite nanomaterials based on Bi and Si produced using laser ablation in liquid followed by subsequent powder annealing. Two synthesis approaches were used, with and without laser post-treatment of mixed (in an atomic ratio of 2:1) laser-generated Bi and Si colloids. A range of methods were used to characterize the samples: UV-Vis diffusion reflection, IR and Raman spectroscopy, synchronous thermal analysis, X-ray diffraction, transmission electron microscopy, as well as specific surface-area evaluation. We also followed the dynamics of phase transformations, as well as composition, structure and morphology of annealed powders up to 800 °C. When heated, the non-irradiated series of samples proceeded from metallic bismuth, through β-Bi2O3, and resulted in bismuth silicates of various stoichiometries. At the same time, in their laser-irradiated counterparts, the formation of silicates proceeded immediately from the amorphous Bi2SiO5 phase formed after laser treatment of mixed Bi and Si colloids. Finally, we show their ability to decompose persistent organic molecules of Rhodamine B and phenol under irradiation with a soft UV (375 nm) source.
Effect of Glass Composition on Luminescence and Structure of CsPbBr3 Quantum Dots in an Amorphous Matrix
Glass matrix embedding is an efficient way to improve the chemical and thermal stability of the halide perovskite QDs. However, CsPbX3 QDs exhibit distinct optical properties in different glass matrixes, including photoluminescence (PL) peak position, PL peak width, and optical band gap. In this work, the temperature-dependent PL spectra, absorption spectra, high-energy X-ray structure factor S(Q), and pair distribution function (PDF) were integrated to analyze the structural evolution of CsPbBr3 QDs in different glass matrixes. The results show that the lattice parameters and atomic spacing of CsPbBr3 QDs are affected by the glass composition in which they are embedded. The most possibility can be attributed to the thermal expansion mismatch between CsPbBr3 QDs and the glass matrix. The results may provide a new way to understand the effect of the glass composition on the optical properties of CsPbBr3 QDs in a glass matrix.
Unveiling structural evolution of Fe single atom catalyst in nitrate reduction for enhanced electrocatalytic ammonia synthesis
Atomic transition metal–nitrogen–carbon electrocatalysts exhibit outstanding activity in various electrocatalytic reactions. The challenge lies in predicting the structure of the active center, which may undergo changes under applied potential and interact with reactants or intermediates. Advanced characterization techniques, particularly in-situ X-ray absorption spectroscopy (XAS), provide crucial insights into the structural evolution of the metal active center during the reaction. In this study, nitrate reduction to ammonia (NO 3 RR) was selected as a model reaction, and we introduced in-situ XAS to reveal the structural evolution during the catalytic process. A novel single atom catalyst of iron loaded on three-dimensional nitrogen-carbon nanonetwork (designated as Fe SAC/NC) was successfully synthesized. We unraveled the structural transformations occurring as pyrrole-N 4 -Fe transitions to pyrrole-N 3 -Fe throughout the NO 3 RR process. Notably, the Fe SAC/NC catalyst exhibited excellent catalytic activity, achieving a Faradaic efficiency of 98.2% and an ammonia generation rate of 22,515 µg·h −1 ·mg cat −1 at −0.8 V versus reversible hydrogen electrode. Theoretical calculations combined with in-situ spectroscopic characterization showed that pyrrole-N 3 -Fe reduced the energy barrier from *NO to *NHO and improved the selectivity of ammonia. This provides a robust reference for the design of efficient nitrate-to-ammonia synthesis catalysts.
Pearl‐Structure‐Enhanced NASICON Cathode toward Ultrastable Sodium‐Ion Batteries
Based on the favorable ionic conductivity and structural stability, sodium superionic conductor (NASICON) materials especially utilizing multivalent redox reaction of vanadium are one of the most promising cathodes in sodium‐ion batteries (SIBs). To further boost their application in large‐scale energy storage production, a rational strategy is to tailor vanadium with earth‐abundant and cheap elements (such as Fe, Mn), reducing the cost and toxicity of vanadium‐based NASICON materials. Here, the Na3.05V1.03Fe0.97(PO4)3 (NVFP) is synthesized with highly conductive Ketjen Black (KB) by ball‐milling assisted sol‐gel method. The pearl‐like KB branch chains encircle the NVFP (p‐NVFP), the segregated particles possess promoted overall conductivity, balanced charge, and modulated crystal structure during electrochemical progress. The p‐NVFP obtains significantly enhanced ion diffusion ability and low volume change (2.99%). Meanwhile, it delivers a durable cycling performance (87.7% capacity retention over 5000 cycles at 5 C) in half cells. Surprisingly, the full cells of p‐NVFP reveal a remarkable capability of 84.9 mAh g−1 at 20 C with good cycling performance (capacity decay rate is 0.016% per cycle at 2 C). The structure modulation of the p‐NVFP provides a rational design on the superiority of others to be put into practice. Ketjen Black (KB) branch chains encircle the Na3.05V1.03Fe0.97(PO4)3 (NVFP) like wearing “pearl,” making the segregated particles link to access the overall conductivity and activating the unusual structural distortion of FeO6 in NVFP during electrochemical progress, thus stimulating plenty of Na+ de/intercalation at plateau region with reversible phase transition and acquiring a favorable rate performance and durable cycling lifespan under fine volume variation.
A Novel Inorganic Aluminum Phosphate-Based Flame Retardant and Thermal Insulation Coating and Performance Analysis
Currently, most thin-layer expandable coatings are polymer-based, with very few inorganic expandable coatings. Due to the high environmental friendliness of inorganic coatings, studying new types of inorganic coatings is of great significance. A novel amorphous aluminum phosphate-based flame-retardant coating was prepared by modifying it with nano-silica, hollow silica beads, hollow glass microspheres, and boron carbide. A comprehensive study was conducted on the flame retardancy and thermal insulation performance, composition and structural evolution under flame and physical and chemical properties, and the mechanisms of flame retardancy and thermal insulation were elucidated. Large-plate combustion testing, bonding strength testing, XRD, IR, TG-DSC, and SEM testing were all applied in this work. The synergistic effect of the four fillers was very obvious, and a series of AP22XY (nano-silica/silica beads/hollow glass microspheres/boron carbide = 2:2:0:4, 2:2:1:3, 2:2:2:2, 2:2:3:1, 2:2:4:0) coatings were prepared. The change in the ratio of glass microspheres to boron carbide had a significant impact on the composition and structural evolution of the coating, thus reflecting its effectiveness as a flame retardant and thermal insulation. Although decreasing the ratio would promote the formation of borosilicate glass and Al18B4O33 and improve the thermal stability of coatings, the structure inside of the coating, especially the skeleton, would be dense, which is not conducive to thermal insulation. When the ratio of glass microspheres to boron carbide is 3:1, AP2231 shows the best fire resistance. Under the combustion of butane flame at about 1200–1300 °C, the backside temperature reaches a maximum of 226 °C at 10 min, and then the temperature gradually decreases to 175 °C at 60 min. This excellent performance is mainly attributed to three aspects: (1) the foaming and expandability of coatings when exposed to fire, (2) the multiple endothermic reactions the coating undergoes, and (3) the improvement effect of boron carbide. Additionally, AP2231 shows the best bonding performance with a strength of close to 4.5 MPa after combustion, because of the appropriate content matching between borosilicate glass, Al18B4O33, and hollow glass microspheres. The coating has potential application prospects in the construction and transportation fields, such as the protection of structural steel, fire prevention in subways and tunnels, and the prevention of lithium battery fires.
Biophysical analysis of the structural evolution of substrate specificity in RuBisCO
Ribulose 1,5-bisphosphate carboxylase/oxygenase (RuBisCO) is the most abundant enzyme on Earth. However, its catalytic rate per molecule of protein is extremely slow and the binding of the primary substrate, CO₂, is competitively displaced by O₂. Hence, carbon fixation by RuBisCO is highly inefficient; indeed, in higher C3 plants, about 30% of the time the enzyme mistakes CO₂ for O₂. Using genomic and structural analysis, we identify regions around the catalytic site that play key roles in discriminating between CO₂ and O₂. Our analysis identified positively charged cavities directly around the active site, which are expanded as the enzyme evolved with higher substrate specificity. The residues that extend these cavities have recently been under selective pressure, indicating that larger charged pockets are a feature of modern RuBisCOs, enabling greater specificity for CO₂. This paper identifies a key structural feature that enabled the enzyme to evolve improved CO₂ sequestration in an oxygen-rich atmosphere and may guide the engineering of more efficient RuBisCOs.
Structural and mechanical evaluation of a new Ti-Nb-Mo alloy produced by high-energy ball milling with variable milling time for biomedical applications
The main focus of this work is to investigate the impact of varying milling times (2 to 18 h) on the structural and mechanical properties of the developed Ti-Nb-Mo alloy. The morphology, phase composition, microstructure, and mechanical behavior of milled and sintered Ti-25Nb-25Mo alloy samples were characterized systematically using x-ray diffraction, scanning electron microscope, optical microscope, and Vicker microhardness. It was noted that the quantity of the β-Ti phase increased as the milling time increased. After 12 h of milling, the synthesized alloys exhibited a spherical morphology and texture with homogeneous distribution. The milled alloys' structural evolution and morphological changes were found to be dependent on their milling duration. Morphological analysis revealed that the crystallite size and mean pore size decreased when the milling duration increased, reaching minimum values of 51 nm and < 1 μm, after 12 and 18 h respectively. As the milling time increased, the grain size decreased, resulting in an increase in density, microhardness, and elastic modulus. Ti-25Nb-25Mo will presents good anti-wear ability and higher resistance to plastic deformation due to enhanced mechanical characteristics (H/E, and H3/E2). Hence, the developed Ti-25Nb-25Mo alloys with reduced elastic modulus and desirable mechanical properties were found to be a promising option for biomedical applications.
Metastable LaOClx Phase Stabilization as an Effective Strategy for Controllable Chlorination of Ethane into 1,2-Dichloroethane
LaOCl-mediated ethane chlorination into 1,2-dichloroethane offers a promising pathway for low-temperature, large-scale ethane upgrading. However, under Cl2-rich conditions, LaOCl undergoes detrimental chlorination into lanthanum chloride (LaCl3), accompanied by extensive surface hydroxylation. Such severe structural evolution limits the practical application of La-based catalysts under industrially relevant conditions. In this study, an alumina-stabilized La catalyst was prepared via a coprecipitation method. We demonstrated that strong La-O-Al interactions effectively resist structural degradation of La species under reaction conditions, enabling the modified catalyst to maintain exceptional stability under high Cl2 concentrations. At a C2H6/Cl2 ratio of 4:9, the optimized catalyst achieves an ethane conversion of 61%, with 1,2-dichloroethane selectivity sustained above 74% for 12 h without noticeable deactivation. In contrast, the bulk LaOCl counterpart suffers from rapid over-chlorination, shifting product dominance to trichloroethane within 10 h. Advanced spectroscopy characterization reveals that selectivity loss in LaOCl originates from phase collapse into LaCl3, whereas Al2O3 stabilization preserves the metastable LaOClx phase in a highly dispersed state, ensuring selective C–Cl bond formation. These results highlight the critical role of stabilizing metastable oxychloride phases through robust metal oxide interactions, establishing a design framework for rare-earth catalysts in high-concentration chlorine environments.
Insights into the kinetics–morphology relationship of 1-, 2-, and 3D TiNb2O7 anodes for Li-ion storage
Understanding the influence of electrode material’s morphology on electrochemical behavior is of great significance for the development of rechargeable batteries, however, such studies are often limited by the inability to precisely control the morphology of electrode materials. Herein, nanostructured titanium niobium oxides (TiNb 2 O 7 ) with three different morphologies (one-dimensional (1D), two-dimensional (2D), and three-dimensional (3D)) were synthesized via a facile microwave-assisted solvothermal method. The influence of the morphological dimension of TiNb 2 O 7 as electrode material on the electrochemical performance in Li-ion batteries (LIBs) and the underlying correlation with the electrochemical kinetics were studied in detail. 2D TiNb 2 O 7 (TNO-2D) shows a superior rate capability and cycling stability, associated with improved kinetics for charge transfer and Li-ion diffusion, compared to the 1D and 3D materials. Operando X-ray diffraction measurements reveal the structural stability and crystallographic evolution of TNO-2D upon lithiation and delithiation and correlate the Li-ion diffusion kinetics with the lattice evolution during battery charge and discharge. Moreover, carbon-coated TNO-2D achieves enhanced rate capability (205 mAh·g −1 at 50 C) and long-term cycling stability (87% after 1000 cycles at 5 C). This work provides insights into the rational morphology design of electrode materials for accelerated charge transfer and enhanced fast-charging capability, pushing forward the development of electrode materials for high-power rechargeable batteries in future energy storage.
Evolutionary Origins and Functional Diversification of 2′-O-Methyltransferases: Insights from Phylogenetic and Structural Analysis
Ribose 2′-O-methylation (Nm), a key RNA modification, is catalyzed by diverse 2′-O-methyltransferases (2′-O-MTases), yet the evolutionary trajectories of these enzymes remain poorly studied. Here, with a comprehensive collection of functionally validated 2′-O-MTases, we classified them into 11 families based on the distinct methyltransferase (MTase) domains. Homology searches across 198 species identified 6746 proteins, revealing the widespread distribution of 2′-O-MTases across the Tree of Life. Eight MTase domains (e.g., FtsJ, SpoU-methylase) existed both in eukaryotes and prokaryotes, indicating their ancient origin in the Last Universal Common Ancestor (LUCA). In contrast, the AdoMet-MTase, TRM13, and Trm56 domains are lineage-specific. Copy number expansion of most 2′-O-MTase families occurred as life evolved from prokaryotes to eukaryotes, where they might engage in more complex regulation of cell differentiation and development. Domain composition, Ka/Ks ratio, and domain structural analyses showed that purifying selection conserved catalytic domains across most families, despite the frequent integration of auxiliary domains. Notably, the FtsJ family diverged into three deeply separated lineages via remodeling the catalytic pocket, with each lineage specializing in the methylation of mRNA caps, rRNA, or tRNA. These findings illuminate the evolutionary trajectory of 2′-O-MTases, highlighting their ancient multiple origins and functional diversification.