arXiv subjects

Kaveh Edalati

Publications and source records attributed to Kaveh Edalati.

At least 19 recordsLinked to original sources

arXiv2026

Nanolamellar Hybrid High-Entropy Alloys with Superior Micromechanical Properties

Metallic materials with nanolamellar structures, such as pearlitic steels, exhibit high strength with appropriate ductility. Considering the potential ability of such nanolamellar structures to break the traditional strength-ductility trade-off in metallic alloys, this study aims at developing a unique nanolamellar structure with superior micromechanical properties by combining two different high-entropy alloys (HEAs). Al0.1CoCrFeNi with the face-centered cubic (FCC) structure is combined with TiZrHfNbTa with the body-centered cubic (BCC) structure using high-pressure torsion (HPT) of half discs of each alloy. That way, a layered hybrid structure was formed, with layer thickness down to about 61 nm. The BCC/FCC nanolamellar hybrid structure exhibits an exceptional combination of properties with an ultimate tensile strength of 2.4 GPa, a maximum bending strength of 4.0 GPa, and a hardness of 740 Hv, while retaining some ductility/plasticity under both tensile and bending loads. Detailed analyses by synchrotron diffraction, electron microscopy and atom probe tomography suggests that these high strength and hardness, which are superior to those of nanostructured HEAs, result from: (i) extreme grain boundary strengthening from nanograins with a mean size of 22 nm, (ii) presence of defects such as dislocations in FCC and BCC, stacking faults in FCC and twins in FCC, and (iii) interphase hardening from BCC/FCC nanolamellar boundaries with about 30% contribution to the total hardness. This work demonstrates that combining two HEAs using HPT into a defect-rich hybrid nanolamellar composite forms a promising synergy of ultrahigh strength and reasonable ductility/plasticity.

cond-mat.mtrl-sci↗

arXiv2026

Thermal and electrical conductivity of a refractory high-entropy alloy after high-pressure torsion: Electron versus phonon contributions

The equiatomic refractory high-entropy alloy TiZrHfNbTa was processed by high-pressure torsion (HPT) to investigate the effect of nanostructuring and defect engineering on thermal and electrical transport properties. Severe plastic deformation (SPD) via the HPT treatment induces substantial accumulation of dislocations, grain refinement to the nanometer level (average: 40 nm), and partial transformation from the BCC phase to the omega phase. While hardness increases to a steady state with processing, the specific heat capacity exhibits a non-monotonic behavior: it decreases at low strains due to the suppression of low-frequency vibrational modes by dislocations, then partially recovers at high strains due to anharmonic vibrations at newly formed high-angle grain boundaries. Thermal conductivity decreases at low strains but shows a slight recovery at high strains, whereas electrical conductivity decreases monotonically to a steady state without recovery. Analysis using the Wiedemann-Franz law reveals that the electronic contribution dominates thermal transport, while the phononic contribution (limited by the scattering of phonons on defects) is only 11 to 23%, depending on the degree of straining. The contrasting evolution of thermal and electrical conductivity is ascribed to the transition from dislocation-dominated vibrations at low strains to grain boundary-dominated vibrations at high strains, which affects phonons and electrons with different efficiencies.

cond-mat.mtrl-sci↗

arXiv2026

High-entropy perovskites, architectured by s0/d0/d10 cations, as novel electrolytes for solid oxide fuel cells

Solid oxide fuel cells enable efficient conversion of hydrogen into electricity. However, the limited availability of materials for their cathode, anode, and electrolyte remains a concern. This study introduces three high-entropy oxide perovskites as novel electrolyte materials for fuel cells (Ba0.50Sr0.50)(Ti0.33Zr0.33Hf0.33)O3 with s0/d0 cations, (Ba0.50Sr0.50)(Ga0.33In0.33Sn0.33)O3 with s0/d10 cations, and (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 with mixed s0/d0/d10 cations. Through sequential sintering by high-pressure torsion processing and calcination, these perovskites were synthesized and then printed with a thickness of about 6-10 microns on a Ni-SrZr0.5Ce0.4Y0.1O3 substrate as an anode and then coated with Ba0.5La0.5CoO3 as a cathode. Electrochemical analysis and impedance spectroscopy show that (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 with s0/d0/d10 cations exhibits the best performance with negligible current leakage and lowest ohmic resistance, while its maximum power density reaches 0.53 W.cm-2 at 973 K. Complementary synchrotron X-ray absorption and photoelectron spectroscopy analyses indicate that the superior performance of (Ba0.50Sr0.50)(Ti0.33Zr0.33Sn0.33)O3 correlates with its heterogeneous electronic structure characterized by tailored unoccupied d-orbital states, and favorable local metal-oxygen bond lengths and extrinsic oxygen vacancies. This investigation demonstrates the significance of high-entropy perovskites with mixed s0/d0/d10 cations as new rare-earth metal-free ion-conducting electrolytes, particularly for protonic solid oxide fuel cells.

cond-mat.mtrl-sci↗

arXiv2026

Sustainable photocatalytic CO2 conversion using microalgae as a carbon-negative scavenger

Photocatalytic CO2 conversion driven by solar energy is a highly promising approach in addressing rising atmospheric CO2 levels; however, its practical application remains limited by low conversion efficiency. In this study, a new strategy to enhance CO2 reduction toward CO and CH4 is proposed through the employment of microalgae as a sacrificial agent, and the efficiency is compared with conventional CO2 conversion without and with the use of microplastics as sacrificial agents. To realize this strategy, an AB2O6-type high-entropy oxide (HEO), (Cs1/7Ba4/7Bi2/7)(Nb1/2Ta1/2)2O6, with bi-polymorphy of layered perovskite and pyrochlore, is rationally designed. The HEO incorporates alkali metal cesium and alkaline earth metal barium to increase surface basicity for CO2 chemisorption, bismuth with its stereochemically active lone pairs for localized polarization and charge separation, and tantalum and niobium to form octahedral crystalline frameworks for charge transport. The utilization of microalgae during photocatalytic reactions leads to a remarkable enhancement in CO2 conversion compared to catalysis with or without using microplastics, with CO and CH4 production increasing by 10- and 4-fold, respectively, compared to the system using only HEO. These findings not only demonstrate a new family of polymorphic AB2-type HEOs for photocatalysis but also show the potential of microalgae as a sustainable sacrificial agent, offering an environmentally friendly pathway for efficient CO2 capture (through photosynthesis by microalgae) and CO2 conversion (through photocatalysis by HEOs).

physics.chem-ph↗

arXiv2026

Machine learning via artificial neural networks coupled with density functional theory and experiments for thermodynamic optimization of high-entropy alloys for hydrogen storage at room temperature

High-entropy alloys (HEAs) have received considerable attention for hydrogen storage because of their compositional flexibility; however, designing HEAs with optimal thermodynamics is critical. This study employs machine learning via artificial neural networks (ANN) and density functional theory (DFT) to design a novel AB-type TixNb2-xVCrMnFe (x = 0.5-2.0) high-entropy system for hydrogen storage at ambient temperature (A: Ti, V and Nb, and B: Cr, Mn and Fe). Both ANN and DFT predict that the hydride formation enthalpy decreases to negative values with increasing the titanium content. Two alloys with x > 1.5 are predicted to achieve enthalpies within the -25 to -39 kJ/mol range, making them appropriate for room-temperature hydrogen storage. Experiments demonstrate good agreement with the enthalpy predictions, with the Ti-rich alloys showing reversible hydrogen storage with fast kinetics at room temperature. These results provide a framework for reliable use of data analysis and ab initio calculations to explore high-entropy hydrides as hydrogen storage materials.

cond-mat.mtrl-sci↗

arXiv2026

Magnesium-graphene interphase boundaries created by high-pressure torsion enhance hydrogen storage kinetics:Mechanisms and significance of activation energy and frequency factor

A strategy to overcome sluggish hydrogenation/dehydrogenation of magnesium is demonstrated by creating magnesium-graphene interphase boundaries via high-pressure torsion (HPT). HPT reduces the grain size of pure magnesium from 1 mm to 850 nm, with 70% of grain boundaries having high misorientation angles. Graphene addition leads to even finer grain sizes of 10-500 nm with a bimodal morphology. The magnesium-graphene composites exhibit superior kinetics at 623 K while maintaining high air resistance. Kinetic modeling reveals that the rate-controlling mechanism transits from interfacial reaction in coarse-grained magnesium to atomic diffusion in magnesium-graphene nanocomposites. Kissinger analysis shows that the activation energy for hydrogen desorption remains unchanged at 145 +/- 2 kJ/mol, regardless of the presence of grain or interphase boundaries. However, the frequency factor (number of successful attempts to overcome the activation energy) increases with the generation of interfaces, which serve as sites for hydrogen diffusion and heterogeneous metal/hydride nucleation. These findings highlight the impact of interphase boundary engineering via severe plastic deformation for enhancing the kinetics and air resistance of hydrogen storage materials.

cond-mat.mtrl-sci↗

arXiv2026

A sustainable photocatalytic pathway for concurrent hydrogen and value-added chemical production utilizing microalgae as bio-scavenger in water

Microalgae are an abundant bioorganic material source and play a significant role in life on Earth by conducting photosynthesis for carbon dioxide (CO2) capture and its conversion to oxygen (O2). In this study, a combination of microalgae as a negative-CO2-emitting sacrificial agent with the traditional photocatalytic water-splitting process using brookite TiO2, as a model photocatalyst, is introduced as a new strategy to maximize green hydrogen (H2) production while converting microalgae to valuable products, like methane (CH4) and carbon monoxide (CO). The process, under optimal conditions, produces up to 0.990 mmol/g.h of H2 without cocatalyst addition and 3.200 mmol/g.h with platinum (Pt) cocatalyst, which is 13 times higher than the production rate without microalgae. The strategy of using microalgae in photocatalysis has high potential in green H2 production, as it not only eliminates valuable hole sacrificial agents, like alcohol, but also produces other useful compounds, like CH4 and CO. Moreover, this sustainable process contributes to CO2 capture and conversion during microalgae cultivation.

physics.chem-ph↗

arXiv2026

High-Pressure Torsion-Induced Transformation of Adenosine Monophosphate: Insights into Prebiotic Chemistry of RNA by Astronomical Impacts

The origin of life is yet a compelling scientific mystery that has sometimes been attributed to high-pressure impacts by small solar system bodies such as comets, meteoroids, asteroids, and transitional objects. High-pressure torsion (HPT) is an innovative method with which to simulate the extreme conditions of astronomical impacts and offers insights relevant to prebiotic chemistry. In the present study, we investigated the polymerization and stability of adenosine monophosphate (AMP), a key precursor to ribonucleic acid (RNA), in dry and hydrated conditions (10 wt% water) under 6 GPa at ambient and boiling water temperatures. Comprehensive analyses with the use of X-ray diffraction, Raman spectroscopy, Fourier-transform infrared spectroscopy, nuclear magnetic resonance, scanning electron microscopy, and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry revealed no evidence of polymerization, while AMP partly transformed to other organic compounds such as nucleobase-derived fragments of adenine, phosphoribose fragments, dehydrated adenosine, protonated adenosine, and oxidized adenosine. The torque measurements during HPT further highlight the mechanical behavior of AMP under extreme conditions. These findings suggest that, while HPT under the conditions tested does not facilitate polymerization, the formation of various compounds from AMP confirms the significance of astronomical impacts on the prebiotic chemistry of RNA on early Earth. Keywords: Ribonucleic acid (RNA), Origin of life; Phase transformations; Chemical reactions, Small solar system bodies

cond-mat.mtrl-sci↗

arXiv2025

Hydrogen diffusion in TiCr$_2$H$_x$ Laves phases: A combined ab initio and machine-learning-potential study

The kinetics of hydrogen diffusion in C15 cubic and C14 hexagonal TiCr$_2$H$_x$ (0 < $x$ <= 4) Laves-phase hydrogen storage alloys is investigated with density functional theory (DFT) and machine learning interatomic potentials (MLIPs). Generalized solid-state nudged elastic band calculations are conducted based on DFT for all symmetrically inequivalent paths between the first-nearest-neighbor face-sharing interstitial sites. The hydrogen migration barriers are substantially higher for the paths that require breaking a Ti-H bond than for those that require breaking a Cr-H bond. Molecular dynamics (MD) simulations with the MLIPs also demonstrate that hydrogen migration occurs more frequently within the hexagonal rings made of the A$_2$B$_2$ interstitial paths, each requiring the breaking of Cr-H bonds, than along the inter-ring paths. The diffusion coefficients of hydrogen obtained from the MD simulations reveal a non-monotonic dependence on hydrogen concentration, which is more pronounced at lower temperatures. Time-averaged radial distribution functions of hydrogen further show that hydrogen avoids face-sharing positions during diffusion and that the hydrogen occupancy at the second-nearest-neighbor edge-sharing positions increases with increasing hydrogen concentration. The diffusion coefficients of hydrogen within 400-1000 K follow an Arrhenius relationship, with activation barriers consistent with most experimental values. One-order of magnitude overestimation of diffusion coefficients compared with some experiments suggests a substantial impact of hydrogen trapping by defects such as Cr vacancies and Ti anti-sites in non-stoichiometric TiCr$_2$ in experiments.

cond-mat.mtrl-sci↗

arXiv2025

Active high-entropy photocatalyst designed by incorporating alkali metals to achieve d0+d10+s0 cationic configurations and wide electronegativity mismatch

Photocatalytic hydrogen (H2) production and carbon dioxide (CO2) conversion to methane (CH4) are considered promising solutions for reducing CO2 emissions. However, the development of highly active photocatalysts is essential to efficiently drive these reactions without harming the environment. In this study, we introduce a strategy that incorporates elements with both low and high electronegativities into catalysts based on transition metals, thereby enhancing both reactant adsorption and charge transfer. This strategy is implemented in a high-entropy oxide (HEO) by adding cesium, an alkali metal with very low electronegativity, and gallium, a metal with high electronegativity, to transition metals titanium, niobium and tantalum. The resulting oxide, TiNbTaGaCsO9 with a large concentration of oxygen vacancies, exhibits strong light absorption, a low bandgap and a suitable band structure for both hydrogen evolution and CO2 conversion. Compared to HEOs with only d0 or d0+d10 cationic configurations, the synthesized oxide with a wide electronegativity difference and mixed d0+d10+s0 cationic configurations shows significantly higher activity for both H2 and CH4 production, even without using a cocatalyst. These results demonstrate a design strategy for creating highly active HEOs containing alkali metals by taking advantage of the electronegativity mismatch across the periodic table.

cond-mat.mtrl-sci↗

arXiv2025

High-entropy perovskites as new photocatalysts for cocatalyst-free water splitting

The photocatalytic water-splitting process is thermodynamically challenging and requires catalysts with suitable band structures, as well as the presence of supporting cocatalysts. By considering the unique charge carrier mobility in perovskites, this study introduces three new ABO3-type high-entropy perovskites (Ba1/2Sr1/2)(Ti1/3Zr1/3Hf1/3)O3, (Ba1/2Sr1/2)(Ga1/3In1/3Sn1/3)O3 and (Ba1/2Sr1/2)(Ti1/3Zr1/3Sn1/3)O3 for cocatalyst-free photocatalysis. The three catalysts, having a single-phase cubic structure, are designed by considering configurational entropy, tolerance factor, octahedral factor, ionic radius deviation and valence deviation of >1.5R (R: gas constant), 0.9-1.0, 0.4-0.8, >0.3 and >0.3, respectively. The perovskites exhibit similar valence band tops, while their bandgaps vary slightly depending on the composition at the B-site (slightly lower bandgap by including d10 cations). Additionally, all three materials demonstrate effective hydrogen generation without the need for added cocatalysts. This investigation confirms that high-entropy oxide perovskites can offer significant potential for cocatalyst-free photocatalytic reactions.

physics.chem-ph↗

arXiv2025

High-entropy oxide photocatalysts for green ammonia synthesis from nitrogen fixation in water

Ammonia, a critical chemical fertilizer and a potential hydrogen carrier, can be sustainably synthesized from atmospheric nitrogen and water under ambient conditions through photocatalysis. In this study, high-entropy oxides with d0 and mixed d0+d10 cationic configurations are introduced as a new group of catalysts for nitrogen fixation and photocatalytic ammonia production. The oxides exhibit impressive efficiency in ammonia production compared to binary oxides, while the efficiency is improved by using a mixed cationic configuration. It was shown that the incorporation of d10 elements, such as gallium and zinc, boosts the photocatalytic reactions by improving light absorbance, charge separation and charge lifetime. These findings demonstrate the potential of high-entropy oxides as next-generation photocatalysts for green ammonia synthesis, offering an effective alternative to conventional catalytic systems.

physics.chem-ph↗

arXiv2025

Understanding high photocatalytic activity of the TiO2 high-pressure columbite phase by experiments and first-principles calculations

The clean production of hydrogen as a zero-emission fuel can be done using photocatalysis, with TiO2 being one of the most promising photocatalysts. However, the activity of TiO2 anatase and rutile phases is still limited. In this study, an oxygen-deficient high-pressure phase of TiO2, columbite, is stabilized by a high-pressure torsion method. The phase is utilized as an active photocatalyst for hydrogen production, and the mechanism of its high activity is examined using density functional theory (DFT). The activity of columbite appears to be experimentally higher than that of the anatase phase. DFT calculations revealed that columbite does not have a narrow electronic bandgap, but its optical bandgap and light absorbance are improved by oxygen vacancies more significantly compared to anatase. Moreover, the water adsorption energy is higher and the surface activation energy for water splitting on the (101) atomic plane of columbite is lower than that for the active planes of anatase. In conclusion, although columbite is not a low-bandgap semiconductor, its large light absorbance and high surface catalytic activity make it a promising candidate for photocatalytic reactions.

cond-mat.mtrl-sci↗

arXiv2025

Boosting hydrogen and methane formation on a high-entropy photocatalyst by integrating atomic d0/d10 electronic junctions and microscopic P/N heterojunctions

The formation of green energy carriers such as hydrogen (H2) and methane (CH4) via photocatalytic processes provides a clean method for addressing environmental and energy issues. To achieve highly efficient photocatalysts for H2 and CH4 generation, the present work introduces the P/N heterojunctions in a high-entropy oxide (HEO) with d0/d10 electronic junctions. The study uses CuO as a P-type semiconductor and the HEO containing d0 (Ti, Zr, Nb, Ta) and d10 (Zn) cations as an N-type semiconductor. The material exhibits improvements in optical properties, such as light absorption, charge mobility and reduced electron-hole recombination. The integration of two concepts, atomic-scale d0/d10 electronic junctions and micro-scale P/N heterojunctions, leads to enhanced H2 and CH4 production. Particularly after the partial removal of vacancies in the heterojunction, H2 production from photocatalytic water splitting reaches 0.71 mmol/g.h, and CH4 evolution from CO2 conversion reaches 2.40 umol/g.h with 72% selectivity for methanation. The integrated strategy of this study has a high potential in developing active heterostructured catalysts for clean fuel production.

physics.chem-ph↗

arXiv2025

Bulk Nanostructured Zirconia Ceramics with High Hardness and Toughness via Integration of High-Pressure Torsion and Spark Plasma Sintering

Developing nanostructured bulk ceramics is a major challenge when conventional high-temperature sintering is employed for consolidation. In the current investigation, yttria-stabilized zirconia (YSZ) with a composition of ZrO2 - 3 mol% Y2O3 is first treated using high-pressure torsion (HPT) and further consolidated using spark plasma sintering (SPS) to produce a nanostructured bulk sample. The material demonstrates phase transformations from tetragonal to dislocation-decorated monoclinic by HPT and reversely transforms to the tetragonal phase after the SPS process while maintaining a mean grain size of 80 nm and large numbers of dislocations. The consolidated ceramic exhibits a density of 6.07 g/cm3 (99% relative density) with a high hardness of 1500 Hv, which is reasonably consistent with the prediction of the Hall-Petch relationship. Examination of the indented areas during the hardness test confirms the absence of cracks, indicating good fracture toughness (KIC) because of the presence of dislocations, while the sample processed only by SPS and without HPT processing forms numerous cracks by indentation and exhibits low KIC.

cond-mat.mtrl-sci↗

arXiv2025

Influence of interphase boundary coherency in high-entropy alloys on their hydrogen storage performance

High-entropy alloys (HEAs) have potential for storing hydrogen reversibly at room temperature due to their tunable thermodynamics; however, they usually suffer from the issue of difficult activation. This study shows that while interphase boundaries are effective in activating some HEAs, some other dual-phase HEAs still require extra high-temperature activation. To understand why interphase boundaries are not always effective for activation, microstructural features and hydrogen storage performance of six HEAs with dual phases are compared. Detailed analysis confirms that interphase boundaries are effective for hydrogen absorption without the need for activation treatment, provided that: (i) their fraction is high enough, and (ii) they are not coherent. These findings are discussed in terms of free volume and boundary energy. Coherent interphase boundaries are associated with lower free volume and thus do not act as fast hydrogen diffusion paths. Moreover, the boundary energy of coherent boundaries is lower than incoherent boundaries, making them less favorable sites for heterogeneous hydride nucleation. This research thus suggests that the introduction of incoherent interphase boundaries with a proper fraction is a solution for activating hydrogen storage materials.

cond-mat.mtrl-sci↗

arXiv2025

Severe Plastic Deformation of Ceramics by High-Pressure Torsion: Review of Principles and Applications

Ceramics are typically brittle at ambient conditions due to their covalent or ionic bonding and limited dislocation activities. While plasticity, and occasionally superplasticity, can be achieved in ceramics at high temperatures through thermally activated phenomena, creep, and grain boundary sliding, their deformation at ambient temperature and pressure remains challenging. Processing under high pressure via the high-pressure torsion (HPT) method offers new pathways for severe plastic deformation (SPD) of ceramics. This article reviews recent advances in HPT processing of ceramics, focusing primarily on traditional ceramics (e.g., oxides, carbides, nitrides, oxynitrides) and to a lesser extent advanced ceramics (e.g., silicon, carbon, perovskites, clathrates). Key structural and microstructural features of SPD-processed ceramics are discussed, including phase transformations and the generation of nanograins and defects such as vacancies and dislocations. The properties and applications of these deformed ceramics are summarized, including powder consolidation, photoluminescence, bandgap narrowing, photovoltaics, photocatalysis (dye degradation, plastic waste degradation, antibiotic degradation, hydrogen production, CO2 conversion), electrocatalysis, thermoelectric performance, dielectric performance, and ion conductivity for Li-ion batteries. Additionally, the article highlights the role of HPT in synthesizing novel materials, such as high-entropy ceramics (particularly high-entropy oxides), black oxides, and high-pressure polymorphs, which hold promise for energy and environmental applications.

cond-mat.mtrl-sci↗

arXiv2025

Boosting biocompatibility and mechanical property evolution in a high-entropy alloy via nanostructure engineering and phase transformations

High-entropy alloys (HEAs), as multi-component materials with high configurational entropy, have garnered significant attention as new biomaterials; still, their low yield stress and high elastic modulus need to be overcome for future biomedical applications. In this study, nanograin generation is used to enhance the strength and phase transformation is employed to reduce the elastic modulus of a biocompatible Ti-Zr-Hf-Nb-Ta-based HEA. The alloy is treated via the high-pressure torsion (HPT) process, leading to (i) a BCC (body-centered cubic) to omega phase transformation with [101]ω//[011]BCC and [211]omega//[121]BCC through a twining mechanism, (ii) nanograin formation with a mean grain size of 20 nm, and (iii) dislocation generation particularly close to BCC-omega interphase boundaries. These structural and microstructural features enhance hardness, increase tensile strength up to 2130 MPa, achieve tensile elongation exceeding 13%, reduce elastic modulus down to 69 GPa and improve biocompatibility. Additionally, the HEA exhibits improved anodization, resulting in a homogenous distribution of oxide nanotubes on the surface with a smaller tube diameter and a higher tube length compared to pure titanium. These remarkable properties, which are engineered by the generation of defective nanograins and the co-existence of BCC and metastable omega phases, highlight the potential of HEAs treated using severe plastic deformation for future biomedical usage, particularly in the orthopedic sector.

cond-mat.mtrl-sci↗