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共价三嗪框架作为烯基化合物氧化反应催化剂的强碱性形成。

Formation of Strong Basicity on Covalent Triazine Frameworks as Catalysts for the Oxidation of Methylene Compounds.

机构信息

State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy , Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 , People's Republic of China.

University of Chinese Academy of Sciences , Beijing 100049 , People's Republic of China.

出版信息

ACS Appl Mater Interfaces. 2018 Apr 18;10(15):12612-12617. doi: 10.1021/acsami.7b19001. Epub 2018 Apr 9.

Abstract

Porous solid bases are increasingly attractive for applications in green chemistry and heterogeneous catalysis under relatively mild conditions. Here, covalent triazine frameworks (CTFs) were first applied as a support for the porous solid strong bases through a redox process between the base precursor KNO and CTFs, leading to a relatively low calcination temperature (400 °C). As a result, porous organic frameworks possessing ordered microstructures as well as strong basic sites were successfully synthesized. The materials were characterized by X-ray diffraction, Fourier transform infrared, high-resolution transmission electron microscopy, temperature programmed desorption of CO, and so forth. The obtained solid bases displayed remarkable catalytic activity in the aerobic oxidation of methylene compounds, and the yield of fluorenones could reach 93.6% at 120 °C, which was nearly 3 times higher than that of the control catalyst. The current research may present a new idea for the construction of porous organic polymers with strong basicity.

摘要

多孔固体碱在相对温和的条件下在绿色化学和多相催化中的应用越来越受到关注。在此,通过碱前体 KNO 和 CTFs 之间的氧化还原反应,首次将共价三嗪骨架(CTFs)用作多孔固体强碱的载体,从而实现相对较低的煅烧温度(400°C)。结果,成功合成了具有有序微结构和强碱性位的多孔有机骨架。通过 X 射线衍射、傅里叶变换红外、高分辨率透射电子显微镜、CO 程序升温脱附等手段对材料进行了表征。所得到的固体碱在亚甲基化合物的有氧氧化中表现出显著的催化活性,在 120°C 下,芴酮的收率可达 93.6%,几乎是对照催化剂的 3 倍。本研究可能为构建具有强碱性的多孔有机聚合物提供了一个新的思路。

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