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Unveiling the Flexocatalytic Potential of Wide-Bandgap Spinel Oxides: Light-Free Hydrogen Evolution via Strain-Induced Polarization and Oxygen Vacancy Engineering
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Unveiling the Flexocatalytic Potential of Wide-Bandgap Spinel Oxides: Light-Free Hydrogen Evolution via Strain-Induced Polarization and Oxygen Vacancy Engineering

Kuang Yuan Tu, Hsun-Yen Lin, Jyh-Pin ChouJyh Ming Wu
Advanced functional materials, 卷.35(31), 2424279
01/08/2025
Web of Science ID: WOS:001436032900001

摘要

Chemistry Chemistry, Multidisciplinary Chemistry, Physical Materials Science, Multidisciplinary Nanoscience & Nanotechnology Physics, Applied Physics, Condensed Matter Science & Technology Science & Technology - Other Topics Materials Science Physical Sciences Physics Technology
Wide-bandgap spinel oxides, such as ZnAl2O4 (ZAO) and ZnCr2O4 (ZCO), are traditionally limited by poor electron activation under light irradiation, resulting in suboptimal photocatalytic performance. This study investigates a novel approach to overcoming these limitations by leveraging the flexoelectric effect in centrosymmetric porous nanoparticles with wrinkled surfaces. The inhomogeneous strain gradients generated under mechanical force induce flexoelectric polarization, offering a promising pathway to enhance photocatalytic activity. ZAO outperforms ZCO due to the smaller atomic radius of aluminum, allowing greater atomic displacement and higher polarization, which prolongs electron-hole recombination. Oxygen vacancies (O-V) further enhance ZAO performance, with ZAO-200 (annealed at 200 degrees C) achieving the longest carrier lifetime (4.65 ns) and an exceptional hydrogen evolution rate of 3737 mu mol g(-1) h(-1)-206% higher than pristine ZAO-without light stimulation. Density functional theory (DFT) calculations confirm a lower hydrogen evolution reaction (HER) energy barrier for ZAO (Delta G(H) = -0.13 eV) compared to ZCO (1.34 eV) and reveal spontaneous water splitting at O-V sites without energy input. A unique butterfly curve validates flexoelectric potential generation from strain gradients. These findings establish a novel framework for eco-friendly hydrogen production, demonstrating that flexoelectric polarization and O-V engineering can surpass traditional photocatalytic methods in sustainability and efficiency.

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https://doi.org/10.1002/adfm.202424279檢視
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