Light-driven, heterogeneous organocatalysts for C-C bond formation toward valuable perfluoroalkylated intermediates.
Light-driven, heterogeneous organocatalysts for C-C bond formation toward valuable perfluoroalkylated intermediates.
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DOI：
10.1126/sciadv.abc9923
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发表时间：
2020-11
期刊：
影响因子：
13.6
通讯作者：
Prato M
中科院分区：
文献类型：
--
作者：
Filippini G;Longobardo F;Forster L;Criado A;Di Carmine G;Nasi L;D'Agostino C;Melchionna M;Fornasiero P;Prato M
深入分析结构/活性关系有助于合理设计用于有机光催化的改性氮化碳。氮化碳（CN）材料在有机合成中的有利开发需要CN结构的适当微调。在这里，我们提出了一个深入的调查结构/活性关系的CN在光催化全氟烷基化的有机化合物。四种类型的CN轴承微妙的结构差异进行了研究，通过传统的表征技术和创新的核磁共振（NMR）实验，关联不同的结构与基本的机械关系，特别是突出的试剂和催化剂表面之间的卤素键强度的重要性。优化的催化剂表现出优异的性能，具有很宽的反应范围，并能显著地利用自然光引发模型反应。这项工作为建立一种新的方法奠定了平台，用于与医学，农业和材料化学相关的有机合成的非均相光催化剂的开发。
In-depth analysis of structure/activity relationship aids rational design of modified carbon nitride for organophotocatalysis. The favorable exploitation of carbon nitride (CN) materials in photocatalysis for organic synthesis requires the appropriate fine-tuning of the CN structure. Here, we present a deep investigation of the structure/activity relationship of CN in the photocatalytic perfluoroalkylation of organic compounds. Four types of CN bearing subtle structural differences were studied via conventional characterization techniques and innovative nuclear magnetic resonance (NMR) experiments, correlating the different structures with the fundamental mechanistic nexus and especially highlighting the importance of the halogen bond strength between the reagent and the catalyst surface. The optimum catalyst exhibited an excellent performance, with a very wide reaction scope, and could prominently trigger the model reaction using natural sunlight. The work lays a platform for establishing a new approach in the development of heterogeneous photocatalysts for organic synthesis related to medical, agricultural, and material chemistry.
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