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可见光催化氢气生成:层状钛酸盐在夹层空间中嵌入钌三(联吡啶)和甲紫精作为光催化剂。

Visible-light hydrogen generation using as photocatalysts layered titanates incorporating in the intergallery space ruthenium tris(bipyridyl) and methyl viologen.

机构信息

Instituto Universitario de Tecnología Química CSIC-UPV, Universidad Politécnica de Valencia, 46022 Valencia, Spain.

出版信息

J Colloid Interface Sci. 2010 Jun 1;346(1):172-7. doi: 10.1016/j.jcis.2010.02.056. Epub 2010 Mar 2.

Abstract

A series of layered titanates containing in the interlayer space tris(2,2'-bipyridyl)ruthenium(II) [Ru(bpy)(3)(2+)] or methyl viologen (MV(2+)) or both has been prepared and characterized by elemental analyses, XRD, and optical and vibrational spectroscopy. Incorporation of Ru(bpy)(3)(2+) and MV(2+) is confirmed by the increase of the distance between the titanate layers. The presence of Ru(bpy)(3)(2+) in the material is also revealed in optical spectroscopy where the ligand to metal charge transfer band appearing at λ(max) 460 nm is observed. Also incorporation of MV(2+) leads to the observation of the charge transfer complex band with the titanate host from 350 to 650 nm. These solids are active for the photocatalytic hydrogen generation from water when colloidal platinum as catalyst and EDTA as sacrificial electron donor are present in the solution. The maximum efficiency was obtained for a solid consisting of layered titanate containing a 10.2 wt.% loading of Ru(bpy)(3)(2+) incorporated in the titanate layers and MV(2+) and Pt nanoparticles in the aqueous solution. This heterogeneous system produced about one-half the hydrogen generated for the conventional homogeneous system where all the components [Ru(bpy)(3)(2+), MV(2+), Pt, and EDTA] are in solution, with the advantage that it can be used as film or recovered by filtration from the aqueous medium.

摘要

一系列层状钛酸盐在层间空间中含有三(2,2'-联吡啶)钌(II)[Ru(bpy)(3)(2+)]或甲紫(MV(2+))或两者均已被制备并通过元素分析,XRD 和光学及振动光谱进行了表征。通过钛酸盐层之间距离的增加确认了 Ru(bpy)(3)(2+)和 MV(2+)的掺入。在光学光谱中也发现了材料中存在 Ru(bpy)(3)(2+),其中观察到出现在 λ(max)460nm 的配体到金属电荷转移带。此外,MV(2+)的掺入导致观察到与钛酸盐主体的电荷转移络合物带,从 350nm 到 650nm。当胶体铂作为催化剂并且 EDTA 作为牺牲电子供体存在于溶液中时,这些固体对于水的光催化析氢是活跃的。在包含层状钛酸盐的固体中获得了最大效率,该固体含有 10.2wt.%的 Ru(bpy)(3)(2+)负载量,Ru(bpy)(3)(2+)掺入钛酸盐层中,并且 MV(2+)和 Pt 纳米颗粒存在于水溶液中。该多相体系产生的氢气约为常规均相体系产生的氢气的一半,其中所有组分[Ru(bpy)(3)(2+),MV(2+),Pt 和 EDTA]均在溶液中,其优点是可以用作薄膜或从水介质中通过过滤回收。

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