Ru(bpy)32+/TiO2-codoped zeolites:: Synthesis, characterization, and the role of TiO2 in electron transfer photocatalysis
Ru(bpy)32+/TiO2-codoped zeolites:: Synthesis, characterization, and the role of TiO2 in electron transfer photocatalysis
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DOI：
10.1021/jp002480m
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发表时间：
2001-06-14
影响因子：
3.3
通讯作者：
Wörner, M
中科院分区：
文献类型：
--
作者：
Bossmann, SH;Turro, C;Wörner, M
开发了新型多相光催化剂，其能够将电子从沸石框架内的激发态Ru（II）供体转移到外部的Co（III）受体络合物。通过元素分析、电化学方法、漫反射、光栅和透射电子显微镜制备并表征了这些材料。该催化剂由Y型沸石包封的Ru（bpy）（3）（2+）（bpy = 2，2 ' -联吡啶）敏化剂与相同载体上的TiO 2纳米颗粒紧密相邻组成。研究了Ru（bpy）（3）（2+）和TiO 2负载量对Ru（bpy）（3）（2+）在沸石超笼中的物理化学性质的影响。Ru（bpy）（3）（2+）的光激发MLCT态通过电子转移与Co（dpphen）（3）（3+）（dpphen = 4，7-二苯基-1，10-菲咯啉）在沸石颗粒外部发生反应。随着沸石中TiO 2含量的增加，Ru（bpy）（3）（2+）被外部Co（dpphen）（3）（3+）的相对猝灭增强，其中来自沸石内部的Ru（bpy）32+络合物的电子转移能够将电子转移到Co（dpphen）（3）（3+）。这一观察结果表明，在适当的电子中继器（如TiO 2纳米颗粒）存在下，电子可以从沸石内部传输到表面。
Novel heterogeneous photocatalysts were developed which are able to transfer electrons from excited Ru(II) donors within the zeolite framework to Co(III) acceptor complexes in the exterior. The materials were prepared and characterized by elemental analysis, electrochemical methods, diffuse reflectance, and raster and transmission electron microscopy. The catalysts consist of zeolite Y-encapsulated Ru(bpy)(3)(2+) (bpy = 2,2 ' -bipyridine) sensitizers in close proximity to TiO2 nanoparticles on the same support. The photophysical properties of Ru(bpy)(3)(2+) within the zeolite supercages were investigated at different loadings of Ru(bpy)(3)(2+) and TiO2. The photoexcited MLCT state of the zeolite-entrapped Ru(bpy)(3)(2+) reacts via electron transfer with Co(dpphen)(3)(3+) (dpphen = 4,7-diphenyl-1,10-phenanthroline) in the exterior of the zeolite particles. The relative quenching of Ru(bpy)(3)(2+) by external Co(dpphen)(3)(3+) increases as the TiO2 content within the zeolite is increased, where electron transfer from Ru(bpy)32+ complexes within the interior of the zeolite are able to transfer electrons to Co(dpphen)(3)(3+). This observation indicates that electrons can be transported from the interior of the zeolite to the surface in the presence of an appropriate electron relay, such as TiO2 nanoparticles.