Highly selective Pd@mpg-C3N4 catalyst for phenol hydrogenation in aqueous phase
Highly selective Pd@mpg-C3N4 catalyst for phenol hydrogenation in aqueous phase
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用于水相苯酚加氢的高选择性 Pd@mpg-C3N4 催化剂
DOI：
10.1039/c3ra41397g
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发表时间：
2013-01-01
期刊：
影响因子：
3.9
通讯作者：
Wang, Yong
中科院分区：
文献类型：
--
作者：
Li, Yi;Xu, Xuan;Wang, Yong
研究了高分子介孔石墨氮化碳（mpg-C3 N4）负载钯催化剂（Pd@ mpg-C3 N4）上苯酚液相选择加氢制环己酮的反应。该Pd@ mpg-C3 N4显示出高活性，并促进在“一步法”中选择性地形成环己酮（类似于99%），环己酮是一种工业上重要的化合物。不同的变量，如溶剂，反应温度，催化剂纹理和催化剂预处理的影响，并进行了讨论。mpg-C3 N4在苯酚和环己酮之间的不同吸附容量被建议强烈促进苯酚化学选择性还原为环己酮，并避免环己酮深度加氢为环己醇。加氢反应动力学可用准一级动力学模型描述，并通过同位素示踪和过渡态计算对反应机理进行了讨论。
The liquid phase selective hydrogenation of phenol to cyclohexanone has been investigated over polymeric mesoporous graphitic carbon nitride (mpg-C3N4) supported Pd catalysts (Pd@mpg-C3N4). This Pd@mpg-C3N4 is shown to be highly active and promotes the selective formation of cyclohexanone (similar to 99%), an industrially important compound, in a "one-step'' method. The effects of different variables like solvent, reaction temperature, catalyst texture and catalyst pre-treatment are presented and discussed. The different adsorption capacity of mpg-C3N4 between the phenol and cyclohexanone is suggested to strongly promote the chemoselective reduction of phenol to cyclohexanone and avoid the deep hydrogenation of cyclohexanone to cyclohexanol. The hydrogenation kinetics has been adequately represented by a standard pseudo-first-order approximation, and isotopic tracing study and the transition state calculation were applied for the discussion of the possible reaction mechanism.