Efficient Aliphatic C-H Oxidation and C=C Epoxidation Catalyzed by Porous Organic Polymer-Supported Single-Site Manganese Catalysts
Efficient Aliphatic C-H Oxidation and C=C Epoxidation Catalyzed by Porous Organic Polymer-Supported Single-Site Manganese Catalysts
复制标题
多孔有机聚合物负载单中心锰催化剂催化高效脂肪族C-H氧化和C=C环氧化
DOI：
10.1021/acscatal.1c02738
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发表时间：
2021
期刊：
影响因子：
12.9
通讯作者：
Sun Wei
中科院分区：
文献类型：
--
作者：
Wang Bingyang;Lin Jin;Sun Qiangsheng;Xia Chungu;Sun Wei
近几十年来，生物启发的锰络合物已成为许多选择性氧化反应的有吸引力的催化剂。然而，这些催化剂仍然受到氧化降解的影响。在本研究中，我们制备了一系列多孔Mn-N4催化剂，其中的催化单元嵌入在多孔有机聚合物(POPS)的骨架中。这些POP基锰催化剂在脂肪族C-H键的氧化和烯烃的不对称环氧化反应中表现出较高的反应活性。此外，由于这些催化剂的非均相性质，它们可以很容易地回收和重复使用。形态表征表明，Mn-N4络合物分散在多孔性聚合物网络中。值得注意的是，单位催化剂的性质防止了反应过程中的氧化降解。因此，本工作成功地开发了一种生物启发的单位锰催化剂，其中的氧化反应以类似酶的方式被限制在特定的通道中。
Bioinspired manganese complexes have emerged over recent decades as attractive catalysts for a number of selective oxidation reactions. However, these catalysts still suffer from oxidative degradation. In the present study, we prepared a series of porous Mn–N4 catalysts in which the catalytic units are embedded in the skeleton of porous organic polymers (POPs). These POP-based manganese catalysts demonstrated high reactivity in the oxidation of aliphatic C–H bonds and the asymmetric epoxidation of olefins. Furthermore, these catalysts could be readily recycled and reused due to their heterogeneous nature. Morphological characterization revealed that the Mn–N4 complex was individually distributed over a porous polymer network. Remarkably, the nature of the single-site catalyst prevented oxidative degradation during the reaction. The present work has thus developed a successful approach for bioinspired single-site manganese catalysts in which the oxidation reaction is confined to a specific channel in an enzyme-like mode.