Liu Chunyao, Wang Changhua, Wang Rui, Li Dashuai, Jin Dexin, Ohtani Bunsho, Liu Baoshun, Ma He, Du Jinglun, Liu Yichun, Zhang Xintong
Key Laboratory of UV-Emitting Materials and Technology of Chinese Ministry of Education, Northeast Normal University, Changchun 130024, China.
Graduate School of Environmental Science, Hokkaido University, Sapporo 060-0810, Japan.
ACS Appl Mater Interfaces. 2024 Sep 11;16(36):48649-48659. doi: 10.1021/acsami.4c10977. Epub 2024 Aug 27.
Surface disordering has been considered an effective strategy for tailoring the charge separation and surface chemistry of semiconductor photocatalysts. A simple but reliable method to create surface disordering is, therefore, urgently needed for the development of high-performance semiconductor photocatalysts and their practical applications. Herein, we report that the ultrasonic processing, which is commonly employed in the dispersion of photocatalysts, can induce the surface disordering of TiO and significantly promote its performance for photocatalytic hydrogen evolution. A 40 min ultrasonic treatment of TiO (Degussa P25) enhances the photocatalytic hydrogen production by 42.7 times, achieving a hydrogen evolution rate of 1425.4 μmol g h without any cocatalyst. Comprehensive structural, spectral, and electrochemical analyses reveal that the ultrasonic treatment induces the surface disordering of TiO, and consequently reduces the density of deep electron traps, extends the separation of photogenerated charges, and facilitates the hydrogen evolution reaction relative to oxygen reduction. The ultrasonic treatment manifests a more pronounced effect on disordering the surface of anatase than rutile, agreeing well with the enhanced photocatalysis of anatase rather than rutile. This study demonstrates that ultrasonic-induced surface disordering could be an effective strategy for the activation of photocatalysts and might hold significant implications for the applications in photocatalytic hydrogen evolution, small molecule activation, and biomass conversion.
表面无序化被认为是一种调整半导体光催化剂电荷分离和表面化学性质的有效策略。因此，迫切需要一种简单可靠的方法来实现表面无序化，以推动高性能半导体光催化剂的开发及其实际应用。在此，我们报道了一种常用于光催化剂分散的超声处理方法，它可以诱导TiO₂的表面无序化，并显著提高其光催化析氢性能。对TiO₂（德固赛P25）进行40分钟的超声处理，可使光催化产氢量提高42.7倍，在无任何助催化剂的情况下实现了1425.4 μmol g⁻¹ h⁻¹的析氢速率。综合的结构、光谱和电化学分析表明，超声处理诱导了TiO₂的表面无序化，从而降低了深电子陷阱的密度，延长了光生电荷的分离，并促进了相对于氧还原的析氢反应。超声处理对锐钛矿型TiO₂表面无序化的影响比对金红石型更为显著，这与锐钛矿型而非金红石型光催化活性的增强相一致。本研究表明，超声诱导的表面无序化可能是一种激活光催化剂的有效策略，对光催化析氢、小分子活化和生物质转化等应用可能具有重要意义。
