Step-by-step fabrication of porphyrin-fullerene supramolecular assemblies and their photoelectrochemical properties
Step-by-step fabrication of porphyrin-fullerene supramolecular assemblies and their photoelectrochemical properties
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DOI：
10.1021/jp711180m
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发表时间：
2008-05-01
影响因子：
3.7
通讯作者：
Yamada, Sunao
中科院分区：
文献类型：
--
作者：
Matsuoka, Ken-Ichi;Akiyama, Tsuyoshi;Yamada, Sunao
采用分步组装、自组装和表面溶胶-凝胶法在氧化铟锡（ITO）衬底上成功制备了卟啉-富勒烯C-60多层膜。首先，半胱胺自组装在ITO表面，然后通过N-H加成反应形成C-60层。分层的C-60进一步与1，2-二氨基乙烷进行另一次N-H加成，以能够形成随后的C-60层，得到双层C-60膜。同时，用2-氨基乙醇处理层状C-60以在C-60层上植入羟基，这对于促进与丁醇钛（IV）的表面溶胶-凝胶反应以植入氧化钛层是必不可少的。然后，通过随后的表面溶胶-凝胶反应，将四羧基苯基卟啉叠加在氧化钛层上。通过重复这些表面溶胶-凝胶反应，卟啉层进一步组装在最外层上。因此，卟啉和C-60多层膜可以通过上述一系列逐步反应来制造。吸收，荧光，石英晶体微天平，和光电化学进行了调查。相当大的光致电子转移之间的光激发卟啉C-60被验证，即使在存在的氧化钛连接层。观察到从多层膜产生可观的光电流，并描述其机制。
Porphyrin-fullerene C-60 multilayered films have been successfully fabricated on an indium-tin-oxide (ITO) substrate by step-by-step, self-assembling, and surface sol-gel processes. First, cysteamine was self-assembled on the ITO surface, and then a C-60 layer was formed via N-H addition reaction. The layered C-60 further underwent another N-H addition with 1,2-diaminoethane to enable formation of the subsequent C-60 layer, giving a double-layered C-60 film. Meanwhile, the layered C-60 was treated with 2-aminoethanol to implant hydroxy groups on the C-60 layer, which was essential to promote the surface sol-gel reaction with titanium(IV) butoxide for implanting the titanium oxide layer. Then tetracarboxyphenylporphyrin was superimposed on the titanium oxide layer by the subsequent surface sol-gel reaction. By repeating these surface sol-gel reactions, the porphyrin layer was further assembled on the outermost layer. Accordingly, the porphyrin and C-60 multilayered films could be fabricated by the series of above-described step-by-step reactions. Absorption, fluorescence, quartz crystal microbalance, and photoelectrochemical investigations were carried out. Considerable photoinduced electron transfer between photoexcited porphyrin to C-60 was verified, even in the presence of the titanium oxide linking layer. Appreciable photocurrent generation from the multilayered films was observed, and its mechanism is described.