Photooxidation of olefins under oxygen in platinum(II) complex-loaded mesoporous molecular sieves

Photooxidation of olefins under oxygen in platinum(II) complex-loaded mesoporous molecular sieves
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DOI:
10.1021/ja0648256
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发表时间:
2006-11-15
影响因子:
15
通讯作者:
Tung, Chen-Ho
Tung, Chen-Ho
中科院分区:
化学1区
文献类型:
--
作者:
Feng, Ke;Zhang, Ren-Yuan;Tung, Chen-Ho

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环化铂(II)配合物已被成功地引入到(3-氨丙基)三乙氧基硅烷修饰的具有大孔六方孔道的有序介孔二氧化硅SBA-15的孔道中。O-1(2)生成的研究表明,当单重态氧(O-1(2))的扩散量子产率为1时,SBA-15纳米孔道中烯烃的富集量是均相溶液中的8倍。在SBA-15孔道中负载的铂(II)络合物是稳定的,并且光敏氧化有效地发生。即使在10次运行后也没有观察到光敏剂的明显降解和浸出。对于昂贵的贵金属催化剂的再循环使用,仅需要简单的过滤。该多功能体系是介孔二氧化硅分子筛中发生光化学反应的一个很好的例子。SBA-15不仅为光敏剂提供了载体,而且还作为纳米反应器促进了光氧化。
Cyclometalated platinum(II) complex has been successfully incorporated into the (3-aminopropyl) triethoxysilane-modified channels of ordered mesoporous silica SBA-15 that has large pore hexagonal channels. Studies on the O-1(2) generation conclusively demonstrates that the olefins in the nano-channels of SBA-15 can be enriched 8 times higher than those in the homogeneous solution as the diffusion quantum yield of singlet oxygen (O-1(2)) is assumed to be unit. The platinum( II) complex loaded in the channel of SBA-15 is stable, and the photosensitized oxidation occurs efficiently. No obvious degradation and leaching of photosensitizers is observed even after 10 runs. Only a simple filtration is needed for the recycled use of the expensive noble metal catalysts. This versatile system is a good example of photochemical reactions occurring in the mesoporous silica molecular sieve. SBA-15 not only provides a support for the photosensitizer, but also acts as a nano-reactor to facilitate the photooxidation.