Hollow anatase TiO2 tetrakaidecahedral crystals with an active {001}/{110} redox interface toward high-performance photocatalytic activity,Chemical Science

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Hollow anatase TiO2 tetrakaidecahedral crystals with an active {001}/{110} redox interface toward high-performance photocatalytic activity
Chemical Science ( IF 7.6 ) Pub Date : 2023-12-05 , DOI: 10.1039/d3sc04328b
Liming Sun ₁ , Yaya Yuan ₁ , Xiaoxiao He ₂ , Wenwen Zhan ₁ , Dong Li ₂ , Yanli Zhao ₃ , Xiao-Jun Wang ₁ , Xiguang Han ₁

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The existence of the oxidation/reduction interface can promote the performance of a photocatalyst, due to its effect on the separation of photogenerated carriers and the surface reactivity. However, it is difficult to construct two sets of oxidation/reduction interfaces in a single crystal and compare their separation efficiency for photogenerated carriers. Introducing a high proportion of active facets into the co-exposed facets is even more challenging. Herein, a hollow anatase TiO₂ tetrakaidecahedron (HTT) with two sets of oxidation/reduction interfaces ({001}/{101} and {001}/{110}) is synthesized by directional chemical etching. Theoretical and experimental results indicate that the {001}/{110} interface is a dominant oxidation/reduction interface, showing a better promotion on the separation of photogenerated carriers than the {001}/{101} interface. In the HTT, the ratio of dominant {001}/(110) is increased and the proportion of the active {110} facet is about 40% (generally about 15%). Therefore, the HTT shows excellent catalytic activity for photocatalytic reductive (hydrogen production) and oxidative (selective oxidation of sulfides) reactions. The HTT also demonstrates favorable photocatalytic activity for the cross-dehydrogenative coupling reaction, where both photogenerated electrons and photogenerated holes are involved, further verifying its high separation efficiency of photogenerated carriers and surface reactivity. This work provides an important guideline for developing advanced structures with a predetermined interface toward desired applications.

中文翻译：

具有活性{001}/{110}氧化还原界面的空心锐钛矿型TiO2十四面体晶体，具有高性能光催化活性

氧化/还原界面的存在可以促进光催化剂的性能，因为它对光生载流子的分离和表面反应活性有影响。然而，在单晶中构建两组氧化/还原界面并比较它们对光生载流子的分离效率是很困难的。将高比例的活性面引入到共同暴露的面中更具挑战性。本文通过定向化学刻蚀合成了具有两组氧化/还原界面（{001}/{101}和{001}/{110}）的中空锐钛矿型TiO ₂十四面体（HTT）。理论和实验结果表明，{001}/{110}界面是主要的氧化/还原界面，比{001}/{101}界面更能促进光生载流子的分离。在HTT中，占主导地位的{001}/(110)的比例增加，并且活跃的{110}面的比例约为40％(通常约为15％)。因此，HTT对光催化还原（制氢）和氧化（硫化物的选择性氧化）反应表现出优异的催化活性。 HTT还对涉及光生电子和光生空穴的交叉脱氢偶联反应表现出良好的光催化活性，进一步验证了其光生载流子的高分离效率和表面反应活性。这项工作为开发具有针对所需应用的预定接口的先进结构提供了重要的指导。

更新日期：2023-12-05

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