Surface self-modification of TiO2 for enhanced photocatalytic toluene oxidation via photothermal effect

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Jinyu Li , Sunzai Ke , Jiayu Yi , Xiang Li , Lijuan Shen , Ruidan Zhang , Min-Quan Yang
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Abstract

Surface modification plays an important role in extending light absorption and enhancing the catalytic performance of semiconductor photocatalysts. However, most current studies focus on pre-modification of the semiconductors before reaction, while surface self-modification of catalyst during photocatalytic reaction process is often neglected. Here, we report the surface self-modification of TiO2 catalyst during photocatalytic oxidation of toluene under UV light irradiation, which changes the colour of TiO2 from white to yellow, and effectively extends its light absorption range into visible light region. The absorbed visible light is primarily released as thermal energy, significantly increasing the temperature of the catalytic system. Mechanistic studies reveal that the temperature elevation facilitates the separation of photogenerated charge carriers in TiO2 and promotes the generation of •O2, consequently accelerating the surface redox reactions. The surface self-modified TiO2 exhibits an enhanced photothermal catalytic benzaldehyde generation of 4485 μmol g−1 h−1 under UV–visible light irradiation, which surpasses the UV-driven activity by a factor of 1.9. This study offers new perspectives on the surface modification of semiconductor photocatalysts during organic transformations. It is anticipated to trigger increased research attention to this effect, ultimately advancing solar-to-chemical energy conversion.

Abstract Image

Abstract Image

通过光热效应对 TiO2 进行表面自修饰以增强其光催化甲苯氧化能力
表面改性在延长半导体光催化剂的光吸收和提高其催化性能方面发挥着重要作用。然而,目前大多数研究都集中在反应前对半导体的预改性,而催化剂在光催化反应过程中的表面自改性往往被忽视。在此,我们报告了在紫外光照射下,TiO2 催化剂在光催化氧化甲苯过程中的表面自改性,这种改性使 TiO2 的颜色从白色变为黄色,并有效地将其光吸收范围扩展到可见光区域。吸收的可见光主要以热能的形式释放出来,显著提高了催化系统的温度。机理研究表明,温度升高有利于 TiO2 中光生电荷载流子的分离,促进 -O2- 的生成,从而加速表面氧化还原反应。在紫外-可见光照射下,表面自修饰的 TiO2 表现出增强的光热催化苯甲醛生成能力,达到 4485 μmol g-1h-1,比紫外光驱动的 TiO2 活性高出 1.9 倍。这项研究为有机物转化过程中半导体光催化剂的表面改性提供了新的视角。预计该研究将引发对这一效应的更多关注,最终推动太阳能到化学能的转换。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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