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Photocatalytic CO_2 reduction over SrTiO_3: Correlation between surface structure and activity

机译：SrTiO_3上的光催化CO_2还原：表面结构与活性之间的关系

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摘要

Perovskite oxide SrTiO3 is a promising semiconductor photocatalyst for CO2 reduction, which has two possible chemical surfaces-TiO2-terminated and SrO-terminated surfaces. Up to now, the effect of chemical surface and its modification on CO2 adsorption, activation and sequential photocatalytic reduction is not established. In the work, SrTiO3, surface-Ti-rich SrTiO3 and Sr(OH)(2)-decorated SrTiO3 were prepared and their structural, surface, and optical properties and photocatalytic activity were explored. It is found that the absorption edge of surface-Ti-rich SrTiO3 shifted toward visible-light region as compared with that of the other two photocatalysts, which is attributed to the decreased Ti 3d ground-state level at the surface. Bicarbonate-(HCO3-) and bidentate carbonate-like (b-CO3=) species are the main species for CO2 adsorption on the surface-Ti-rich SrTiO3, whereas, besides HCO3- and b-CO3=, plenty of monodentate carbonate-like species (m-CO3=) that has relatively low reactivity is present on the SrTiO3 and Sr(OH)(2)-decorated photocatalysts. As a result, the surface-Ti-rich SrTiO3 exhibits the highest activity for CO2 reduction. Furthermore, although Sr(OH)(2)-decoration and SrO-terminated surfaces facilitate CO2 fixing, the produced surface species are attached to the weakly active Sr ions, giving rise to the lower reactivity. The present work might supply a guide for designing highly active perovskite-type semiconductors for photocatalysis. (C) 2018 Elsevier B.V. All rights reserved.
机译：钙钛矿氧化物SrTiO3是用于CO2还原的有前途的半导体光催化剂，它具有两个可能的化学表面-TiO2封端和SrO封端的表面。迄今为止，尚未确定化学表面及其修饰对CO 2吸附，活化和顺序光催化还原的影响。在工作中，制备了SrTiO3，表面富含钛的SrTiO3和装饰有Sr（OH）（2）的SrTiO3，并研究了它们的结构，表面，光学性质和光催化活性。发现与其他两种光催化剂相比，富钛表面的SrTiO3的吸收边缘向可见光区域移动，这归因于表面Ti 3d基态水平的降低。碳酸氢根（HCO3-）和碳酸盐类双齿碳酸盐（b-CO3 =）是富含Ti的SrTiO3表面吸附CO2的主要物种，而除了HCO3-和b-CO3 =之外，还有大量单齿碳酸盐-在SrTiO3和Sr（OH）（2）修饰的光催化剂上存在反应性相对较低的类似物质（m-CO3 =）。结果，表面富钛的SrTiO3表现出最高的CO2还原活性。此外，尽管Sr（OH）（2）修饰和SrO端接的表面有助于CO2固定，但产生的表面物质附着在弱活性Sr离子上，导致较低的反应性。本工作可能会为设计用于光催化的高活性钙钛矿型半导体提供指导。 （C）2018 Elsevier B.V.保留所有权利。

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  • 来源
    《Applied Surface Science》 |2018年第31期|627-635|共9页
  • 作者

    Luo Chao; Zhao Jie; Li Yingxuan; Zhao Wen; Zeng Yubin; Wang Chuanyi;

  • 作者单位

    Wuhan Univ, Hubei Key Lab Accoutrement Tech Fluid Machinery &, Wuhan 430072, Hubei, Peoples R China;

    Shaanxi Univ Sci & Technol, Sch Environm Sci & Engn, Xian 710021, Shaanxi, Peoples R China;

    Shaanxi Univ Sci & Technol, Sch Environm Sci & Engn, Xian 710021, Shaanxi, Peoples R China;

    Wuhan Univ, Hubei Key Lab Accoutrement Tech Fluid Machinery &, Wuhan 430072, Hubei, Peoples R China;

    Wuhan Univ, Hubei Key Lab Accoutrement Tech Fluid Machinery &, Wuhan 430072, Hubei, Peoples R China;

    Shaanxi Univ Sci & Technol, Sch Environm Sci & Engn, Xian 710021, Shaanxi, Peoples R China;

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  • 正文语种 eng
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  • 关键词

    Perovskite oxides; SrTiO3; Ti-rich surface; Photocatalytic CO2 reduction;

    机译：钙钛矿氧化物;SrTiO3;富钛表面;光催化还原CO2;

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