Encapsulation of Nonprecious Metal into Ordered Mesoporous N-Doped Carbon for Efficient Quinoline Transfer Hydrogenation with Formic Acid
Encapsulation of Nonprecious Metal into Ordered Mesoporous N-Doped Carbon for Efficient Quinoline Transfer Hydrogenation with Formic Acid
复制标题
将非贵金属封装到有序介孔氮掺杂碳中用于甲酸高效喹啉转移氢化
DOI：
10.1021/acscatal.8b01404
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发表时间：
2018-09-01
期刊：
影响因子：
12.9
通讯作者：
Huang, Wenyu
中科院分区：
文献类型：
--
作者：
Li, Guoqiang;Yang, Huanhuan;Huang, Wenyu
以[Co（NH 2CH 2CH 2NH 2）2] Cl 2和四氯化碳为原料，采用硬模板法制备了包覆Co纳米粒子的有序介孔氮掺杂碳（OMNC）。催化剂（Co@OMNC）在不同温度下热解并通过元素分析、Brunauer-Emmett-Teller（BET）、X射线衍射（XRD）、X射线光电子能谱（XPS）和透射电子显微镜（TEM）表征。在无碱条件下以甲酸（FA）为氢源的喹啉转移氢化反应中，包封的Co NP与酸性反应溶液物理隔离，这防止了它们中毒或浸出。丰富的介孔和N掺杂剂提供增强的喹啉吸附。Co@OMNC-700（在700 °C下热解）在140 °C下4小时给出最佳活性（98.8%转化率）以及>99%的1，2，3，4-四氢喹啉（THQ）选择性，与使用H2作为氢化物相比表现出显著改善的性能。
Ordered mesoporous N-doped carbon (OMNC) encapsulating Co nanoparticles (NPs) have been prepared under direct polymerization between [Co(NH2CH2CH2NH2)2]Cl2 and carbon tetrachloride through a hard template method. The catalysts (Co@OMNC) are pyrolyzed at various temperatures and characterized by elemental analysis, Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). In the quinoline transfer hydrogenation with formic acid (FA) as the hydrogen source under a base-free condition, the encapsulated Co NPs are physically isolated from the acidic reaction solution, which prevents them from poisoning or leaching. The rich mesopores and N dopants afford enhanced adsorption of quinoline. Co@OMNC-700 (pyrolyzed at 700 °C) gives the best activity (98.8% conversion) as well as >99% 1,2,3,4-tetrahydroquinoline (THQ) selectivity at 140 °C for 4 h, exhibiting significantly improved performance compared to using H2 as the hydrogenation ...