arXiv subjects

Makoto Arita

Publications and source records attributed to Makoto Arita.

6 recordsLinked to original sources

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

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↗

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↗

arXiv2024

Black brookite rich in oxygen vacancies as an active photocatalyst for CO2 conversion: experiments and first-principles calculations

Photocatalytic CO2 conversion is a clean technology to deal with CO2 emissions, and titanium oxide (TiO2) polymorphs are the most investigated photocatalysts for such an application. In this study, black TiO2 brookite is produced by a high-pressure torsion (HPT) method and employed as an active photocatalyst for CO2 conversion. Black brookite with a large concentration of lattice defects (vacancies, dislocations and grain boundaries) showed enhanced light absorbance, narrowed optical bandgap and diminished recombination rate of electrons and holes. The photocatalytic activity of the black oxide for CO2 conversion was higher compared to commercial brookite and benchmark P25 catalyst powders. First-principles calculations suggested that the presence of oxygen vacancies in black brookite is effective not only for reducing optical bandgap but also for providing active sites for the adsorption of CO2 on the surface of TiO2.

cond-mat.mtrl-sci↗

arXiv2023

Defective high-entropy oxide photocatalyst with high activity for CO2 conversion

High-entropy oxides (HEOs), as a new family of materials with five or more principal cations, have shown promising properties for various applications. In this work and inspired by inherent defective and strained structure of HEOs, photocatalytic CO2 conversion is examined on a dual-phase TiZrNbHfTaO11 synthesized by a two-step high-pressure torsion mechanical alloying and high-temperature oxidation. The HEO, which had various structural defects, showed simultaneous photocatalytic activity for CO2 to CO and H2O to H2 conversion without the addition of a co-catalyst. The photocatalytic activity of this HEO for CO2 conversion was better than conventional photocatalysts such as anatase TiO2 and BiVO4 and similar to P25 TiO2. The high activity of HEO was discussed in terms of lattice defects, lattice strain, light absorbance, band structure, photocurrent generation and charge carrier mobility to activation centers. The current study confirms the high potential of HEOs as a new family of photocatalysts for CO2 conversion.

cond-mat.mtrl-sci↗

arXiv2023

Visible-light photocatalytic oxygen production on a high-entropy oxide by multiple-heterojunction introduction

High-entropy oxides (HEOs), as multi-component ceramics with high configurational entropy, have been of recent interest due to their attractive properties including photocatalytic activity for H2 production and CO2 conversion. However, the photocatalytic activity of HEOs is still limited to ultraviolet light. In this study, to achieve visible-light-driven photocatalysis, 10 different heterojunctions were simultaneously introduced in the Ti-Zr-Nb-Ta-W-O system. The oxide, which was synthesized by a high-pressure torsion method and oxidation, successfully produced oxygen from water under visible light without co-catalyst addition. The photocatalytic performance was attributed to high visible-light absorption, narrow bandgap, appropriate band structure, presence of multiple heterojunctions and accordingly easy electron-hole separation and slow recombination. These results not only show the potential of high-entropy oxides as new visible-light-active photocatalysts, but also introduce the multiple-heterojunction introduction as a strategy to achieve photocatalysis under visible light.

cond-mat.mtrl-sci↗