<br>用于电催化的纳米 TiO2/TiN 系统：绘制半导体|集电体界面能带图的变化以及使用紫外光电子能谱研究 TiO2 电化学还原的影响,ACS Applied Materials & Interfaces

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用于电催化的纳米 TiO2/TiN 系统：绘制半导体|集电体界面能带图的变化以及使用紫外光电子能谱研究 TiO2 电化学还原的影响
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-09-04 , DOI: 10.1021/acsami.4c09736
Beatriz de la Fuente ₁ , Divyansh A Khurana _{2,

3,

4} , Philippe M Vereecken _{2,

3,

4} , Annick Hubin ₁ , Tom Hauffman ₁

Affiliation

TiO ₂是光电催化系统中使用最广泛的材料。了解其在此类系统中的功效的一个关键参数是半导体层中的能带弯曲。在这方面，有关半导体/集流体界面（尤其是纳米半导体电极）的能带能量的知识极其重要，因为它将直接影响其与电解质界面处的任何电荷转移过程。由于在不影响其结构的情况下直接研究界面电子特征是困难的，因此很少尝试专门研究半导体/集流体界面。这项工作利用紫外光电子能谱 (UPS) 确定使用 Ar 气体团簇离子束达到的纳米 TiO ₂ /TiN 薄膜系统中不同深度的价带最大值 ( E _VBM ) 和费米能级 ( E _F ) （GCIB）。通过将 UPS 与 GCIB 深度分析相结合，我们报告了一种创新方法，可以真正绘制纳米半导体/集电器界面上的能带结构。通过将其与X射线光电子能谱(XPS)结合，还可以研究纳米TiO ₂ /TiN界面的化学、化学键合和电子性质之间的相关性。还研究了水性电解质中 TiO ₂原位电化学还原的影响，其中 UPS 证实半导体功函数 (WF) 降低，并且纳米 TiO ₂电极在用于电池后 n 型 Ti ³⁺中心相关增加。 0.2 M 氯化钾溶液。我们报告了使用 UPS 精确确定纳米 TiO ₂ /TiN 薄膜界面的能带图，并确认了电催化过程中 TiO ₂ n 型掺杂剂浓度的增加，从而促进了对纳米 TiO 2 /TiN 薄膜界面的更全面和直观的理解通过质子插层的TiO ₂活化机制，进一步优化了用于太阳能转换的高效光催化材料的设计过程。

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Nano-TiO2/TiN Systems for Electrocatalysis: Mapping the Changes in Energy Band Diagram across the Semiconductor|Current Collector Interface and the Study of Effects of TiO2 Electrochemical Reduction Using UV Photoelectron Spectroscopy

TiO₂ is the most widely used material in photoelectrocatalytic systems. A key parameter to understand its efficacy in such systems is the band bending in the semiconductor layer. In this regard, knowledge on the band energetics at the semiconductor/current collector interface, especially for a nanosemiconductor electrode, is extremely vital as it will directly impact any charge transfer processes at its interface with the electrolyte. Since direct investigation of interfacial electronic features without compromising its structure is difficult, only seldom are attempts made to study the semiconductor/current collector interface specifically. This work utilizes ultraviolet photoelectron spectroscopy (UPS) to determine the valence band maximum (E_VBM) and Fermi level (E_F) at different depths in a nano-TiO₂/TiN thin-film system reached using an Ar gas-clustered ion beam (GCIB). By combining UPS with GCIB depth profiling, we report an innovative approach for truly mapping the energy band structure across a nanosemiconductor/current collector interface. By coupling it with X-ray photoelectron spectroscopy (XPS), correlations among chemistry, chemical bonding, and electronic properties for the nano-TiO₂/TiN interface could also be studied. The effects of TiO₂ in situ electrochemical reduction in aqueous electrolytes are also investigated where UPS confirmed a decrease in the semiconductor work function (WF) and an associated increase in n-type Ti³⁺ centers of nano-TiO₂ electrodes post use in a 0.2 M potassium chloride solution. We report the use of UPS to precisely determine the energy band diagrams for a nano-TiO₂/TiN thin-film interface and confirm the increase in TiO₂ n-type dopant concentrations during electrocatalysis, promoting a much more comprehensive and intuitive understanding of the TiO₂ activation mechanism by proton intercalation and therefore further optimizing the design process of efficient photocatalytic materials for solar conversion.

更新日期：2024-09-04

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