Enhanced Photoanodic Activity and Outermost Surface Crystallinity of Tungsten Oxide via High-temperature Sintering

IF 2.7 4区化学 Q3 CHEMISTRY, PHYSICAL Electrocatalysis Pub Date : 2023-12-20 DOI:10.1007/s12678-023-00859-2

Toshiyuki Abe, Hideya Tsuchikado, Mitsuharu Chisaka, Takashi Itoh, Guoqing Guan, Abuliti Abudula

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Abstract

Tungsten oxide (WO₃) is a promising photoanode material capable of water oxidation under visible-light irradiation. Although WO₃ is usually prepared via sintering at 500 °C–550˚C, this work shows that high-temperature sintering (i.e., at 600 °C) can lead to efficient output at the WO₃ photoanode. The material characteristics such as the crystal system, surface structure, film thickness, and optical properties were essentially independent of the sintering temperatures employed. However, the high-temperature-sintered WO₃ showed low charge transfer resistance at the electrode–electrolyte interface, resulting in improved charge injection efficiency for water oxidation at the WO₃ photoanode. WO₃ sintered at 550 °C and 600 °C showed the similar visible Raman spectra with strong band intensities, indicative of improved crystallinity in WO₃ bulk particularly in the comparison with WO₃ sintered at 450 °C. However, the ultraviolet Raman spectrum exhibited intense bands for only the WO₃ prepared at 600 °C, indicating the enhanced crystallization of the WO₃ outermost surface. Thus, the high crystallinity in the WO₃ bulk and at its surface results in efficient photoanodic output owing to the suppression of electron–hole recombination.

Graphical Abstract

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通过高温烧结提高氧化钨的光阳极活性和最外层表面结晶度

摘要氧化钨（WO3）是一种很有前途的光阳极材料，能够在可见光照射下氧化水。虽然 WO3 通常是在 500 ℃-550 ℃ 下烧结制备的，但本研究表明，高温烧结（即 600 ℃）可使 WO3 光阳极产生高效的输出。晶体系统、表面结构、薄膜厚度和光学特性等材料特性基本上与所采用的烧结温度无关。然而，高温烧结的 WO3 在电极-电解质界面上显示出较低的电荷转移电阻，从而提高了 WO3 光阳极上水氧化的电荷注入效率。在 550 °C 和 600 °C 下烧结的 WO3 显示出相似的可见光拉曼光谱，具有较强的带强度，表明 WO3 块体的结晶度有所提高，尤其是与 450 °C 下烧结的 WO3 相比。然而，紫外拉曼光谱只有在 600 ℃ 制备的 WO3 才显示出强烈的条带，表明 WO3 最外层表面的结晶度提高了。因此，由于电子-空穴重组受到抑制，WO3 块体及其表面的高结晶度导致了高效的光阳极输出。图表摘要

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来源期刊

Electrocatalysis CHEMISTRY, PHYSICAL-ELECTROCHEMISTRY

CiteScore

4.80

自引率

6.50%

发文量

审稿时长

>12 weeks

期刊介绍： Electrocatalysis is cross-disciplinary in nature, and attracts the interest of chemists, physicists, biochemists, surface and materials scientists, and engineers. Electrocatalysis provides the unique international forum solely dedicated to the exchange of novel ideas in electrocatalysis for academic, government, and industrial researchers. Quick publication of new results, concepts, and inventions made involving Electrocatalysis stimulates scientific discoveries and breakthroughs, promotes the scientific and engineering concepts that are critical to the development of novel electrochemical technologies. Electrocatalysis publishes original submissions in the form of letters, research papers, review articles, book reviews, and educational papers. Letters are preliminary reports that communicate new and important findings. Regular research papers are complete reports of new results, and their analysis and discussion. Review articles critically and constructively examine development in areas of electrocatalysis that are of broad interest and importance. Educational papers discuss important concepts whose understanding is vital to advances in theoretical and experimental aspects of electrochemical reactions.