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模板合成单晶-like 多孔 SrTiO₃ 纳米立方体组装体及其增强的光催化析氢性能。

Template synthesis of single-crystal-like porous SrTiO₃ nanocube assemblies and their enhanced photocatalytic hydrogen evolution.

机构信息

Department of Chemistry & William Mong Institute of Nano Science and Technology, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

出版信息

ACS Appl Mater Interfaces. 2013 May;5(9):3683-90. doi: 10.1021/am400254n. Epub 2013 Apr 22.

Abstract

Porous nanostructures of semiconductors are well-known for their ability to enhance the photocatalytic activity thanks to the large specific surface area and abundant active sites for the reactions, interfacial transport, and high utilization of light arising from multireflections in the pores. In this paper, we have successfully fabricated a special porous SrTiO3 three-dimensional (3D) architecture through a facile hydrothermal reaction at 150 °C, using layered protonated titanate hierarchical spheres (LTHSs) of submicrometer size as a precursor template. The SrTiO3 architecture is characterized by the 3D assembly of hundreds of highly oriented nanocubes of 60-80 nm by the partial sharing of (100) faces, thereby displaying porous but single-crystal-like features reminiscent of mesocrystals. Our experimental results have shown the key roles played by the template effect akin to that in topotactic transformation in crystallography and Ostwald-ripening-assisted oriented attachment in the formation of such nanocube assemblies. Compared to the solid SrTiO3 photocatalysts previously synthesized by high-temperature solid-state methods, the as-synthesized porous SrTiO3 nanocube assemblies have relatively large specific surface areas (up to 20.83 m(2)·g(-1)), and thus they have exhibited enhanced photocatalytic activity in hydrogen evolution from water splitting. Expectantly, our synthetic strategy using LTHSs as the precursor template may be extended to the fabrication of other titanate photocatalysts with similar porous hierarchical structures by taking advantage of the diversity of the perovskite-type titanate.

摘要

半导体的多孔纳米结构以其能够提高光催化活性而闻名,这要归功于大的比表面积和丰富的反应活性位、界面传输以及由于孔中的多次反射而产生的光的高利用率。在本文中,我们通过在 150°C 下进行简单的水热反应,成功地制备了一种特殊的多孔 SrTiO3 三维(3D)结构,使用亚微米尺寸的层状质子化钛酸盐分级球体(LTHS)作为前体模板。SrTiO3 结构的特点是通过部分共享(100)面,由数百个高度取向的纳米立方体组装而成,纳米立方体的尺寸为 60-80nm,从而显示出多孔但单晶状的特征,类似于准晶。我们的实验结果表明,模板效应在形成这种纳米立方体组装体中起着关键作用,类似于晶体学中的拓扑转变和奥斯特瓦尔德熟化辅助的取向附着。与以前通过高温固态方法合成的固态 SrTiO3 光催化剂相比,合成的多孔 SrTiO3 纳米立方体组装体具有相对较大的比表面积(高达 20.83 m2·g-1),因此在水分解制氢中表现出增强的光催化活性。我们期望,使用 LTHS 作为前体模板的合成策略可以通过利用钙钛矿型钛酸盐的多样性,扩展到其他具有类似多孔分级结构的钛酸盐光催化剂的制备。

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