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通过在 SrTiO 光催化剂中受控镁掺入来促进光催化整体水分解。

Promoting Photocatalytic Overall Water Splitting by Controlled Magnesium Incorporation in SrTiO Photocatalysts.

机构信息

Photocatalytic Synthesis Group, MESA+ Institute for Nanotechnology, Faculty of Science and Technology (TNW), University of Twente, Meander, P.O. Box 217-7500, AE, Enschede, The Netherlands.

Department of Chemistry, National Tsing Hua University, Hsinchu, 30013, Taiwan.

出版信息

ChemSusChem. 2017 Nov 23;10(22):4510-4516. doi: 10.1002/cssc.201701794. Epub 2017 Nov 10.

Abstract

SrTiO is a well-known photocatalyst inducing overall water splitting when exposed to UV irradiation of wavelengths <370 nm. However, the apparent quantum efficiency of SrTiO is typically low, even when functionalized with nanoparticles of Pt or Ni@NiO. Here, we introduce a simple solid-state preparation method to control the incorporation of magnesium into the perovskite structure of SrTiO . After deposition of Pt or Ni@NiO, the photocatalytic water-splitting efficiency of the Mg:SrTiO composites is up to 20 times higher compared to SrTiO containing similar catalytic nanoparticles, and an apparent quantum yield (AQY) of 10 % can be obtained in the wavelength range of 300-400 nm. Detailed characterization of the Mg:SrTiO composites revealed that Mg is likely substituting the tetravalent Ti ion, leading to a favorable surface-space-charge layer. This originates from tuning of the donor density in the cubic SrTiO structure by Mg incorporation and enables high oxygen-evolution rates. Nevertheless, interfacing with an appropriate hydrogen evolution catalyst is mandatory and non-trivial to obtain high-performance in water splitting.

摘要

SrTiO 是一种众所周知的光催化剂,当暴露在 <370nm 的紫外光照射下时,会引发整体水分解。然而,SrTiO 的表观量子效率通常较低,即使用 Pt 或 Ni@NiO 的纳米粒子进行功能化也是如此。在这里,我们引入了一种简单的固态制备方法来控制镁掺入 SrTiO 的钙钛矿结构中。在沉积 Pt 或 Ni@NiO 之后,与含有类似催化纳米粒子的 SrTiO 相比,Mg:SrTiO 复合材料的光催化水分解效率高达 20 倍,并且可以在 300-400nm 的波长范围内获得 10%的表观量子产率 (AQY)。对 Mg:SrTiO 复合材料的详细表征表明,Mg 可能取代四价 Ti 离子,从而形成有利的表面空间电荷层。这源于通过 Mg 掺入来调整立方 SrTiO 结构中的施主密度,并实现高的氧气析出速率。然而,与适当的析氢催化剂相连接是获得高效水分解的必要条件,而且并非微不足道。

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