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首页> 外文期刊>Catalysis science & technology >N/O-doped carbon as a 'solid ligand' for nano-Pd catalyzed biphenyl- and triphenylamine syntheses
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N/O-doped carbon as a 'solid ligand' for nano-Pd catalyzed biphenyl- and triphenylamine syntheses

机译:N / O-doped碳作为nano-Pd“坚实的配体”催化联苯和三苯胺合成

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摘要

A series of N/O-doped porous carbon supported nanopalladium catalysts have been successfully prepared, in which the N/O doped carbons were controllably produced via polypyrrole/furan synthesis followed by carbonization. These catalysts exhibit good performance in biphenylamine and triphenylamine syntheses with nitrobenzene and cyclohexanone as starting materials. Their catalytic activity can be tuned efficiently by the N/O functional groups on the carbon surface. TEM, XRD, XPS and laser Raman methods were applied to probe the structure of these catalysts. These results indicate that the Pd nanoparticles were supported on N/O-doped porous carbon via the "coordination" between Pd nanoparticles and N/O functional groups including O-C=O, C=N and tertiary nitrogen, and better catalytic performance was obtained if carbon with the highest N-species loading was used as the support. In addition, a mechanistic study proved that the reaction starts with the catalytic reduction of nitrobenzene with cyclohexanone as the hydrogen source. During this reaction, aniline was formed and the cyclohexanone was transformed into phenol. Then biphenylamine and triphenylamine were generated through the reaction of aniline and cyclohexanone. This work should facilitate the controllable preparation of carbon supported nanocatalysts with specific activity, and open up a promising pathway for the development of new methodologies for N-containing fine chemical synthesis.
机译:一系列的N / O-doped多孔碳的支持nanopalladium催化剂已成功准备,N / O掺杂碳通过聚吡咯/呋喃可控生产合成碳化紧随其后。催化剂表现出良好的性能联苯胺和三苯胺合成硝基苯和环己酮作为开始材料。有效的N / O的官能团碳表面。方法应用于探测器的结构这些催化剂。钯纳米颗粒在N / O-doped支持多孔碳通过Pd之间的“协调”纳米颗粒和N / O等官能团O C = O、C = N叔氮,更好如果碳与催化性能得到作为最高N-species加载支持。从催化的反应减少硝基苯与环己酮氢的来源。苯胺形成和环己酮转化为酚。三苯胺生成通过苯胺的反应和环己酮。应该促进的可控制备碳nanocatalysts与特定的支持活动,打开一个有前途的途径N-containing开发的新方法精细化工合成。

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