新型可见光催化反应的研究
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摘要
光化学反应是以光为激发手段研究激发态分子的反应。它以洁净、节能、节约为目标,正在成为C-H键活化与官能团化最为活跃的研究领域之一。我们利用可见光催化实现了一系列惰性C-H键活化及官能团的反应,并利用稳态和时间分辨的光谱技术明晰了反应机制。更有意义的是,针对交叉脱氢偶联反应必须在当量氧化剂帮助下有效进行的特点,我们开发了"交叉偶联放氢反应"新反应。在可见光的照射下,无需氧化剂的参与,直接构建了新型的碳-碳键、碳-杂键和硫-硫等杂原子键,并将脱除的电子和质子高效催化转化为氢气放出~([1-4])。"交叉偶联放氢反应"避免了底物的预先官能化,缩短了合成路线,是高效、原子经济性和环境友好的新反应,其特点在大规模工业生产中显得格外重要且必要。
Fascinated by the ability of natural photosynthetic systems to convert solar energy into chemical energy, the scientific community long ago recognized the potential of light-driven reactions(photochemistry) as a powerful approach to chemical synthesis.From the high energy intermediate generated by photoinduced excitation of organic molecules, unique reaction manifolds can be accesses that are generally unavailable to conventional thermal pathways. Thus photochemical reactions considerably enrich the synthetic repertoire of modern organic chemists. Our group has long engaged in the photochemistry research related to the photoinduced energy transfer, electron transfer and chemical transformation. In this presentation, we will report our recent progress on photocatalytic C-H bond activation and functionalization.
引文
[1]Wu,L.-Z.;Chen,B.;Li,Z.-J.;Tung,C.-H.Acc.Chem.Res.2014,47:2177.
    [2]Meng,Q.-Y.;Zhong,J.-J.;Liu,Q.;Gao,X.-W.;Zhang,H.-H.;Lei,T.;Li,Z.-J.;Feng,K.;Chen,B.;Tung,C.-H.;Wu,L.-Z.J.Am.Chem.Soc.2013,135:19052.
    [3]Zhong,J.-J.;Meng,Q.-Y.;Liu,B.;Li,X.-B.;Gao,X.-W.;Lei,T.;Wu,C.-J.;Li,Z.-J.;Tung,C.-H.;Wu,L.-Z.Org.Lett.2014,16:1988.
    [4]Li,X.-B.;Li,Z.-J.;Gao,Y.-J.;Meng,Q.-Y.;Yu,S.;Weiss,R.G.;Tung,C.-H.;Wu,L.-Z.Angew.Chem.Int.Ed.2014,53:2085.

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