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首页> 外文期刊>ACS catalysis >Nitrogen-Functionalized Ordered Mesoporous Carbons as Multifunctional Supports of Ultrasmall Pd Nanoparticles for Hydrogenation of Phenol
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Nitrogen-Functionalized Ordered Mesoporous Carbons as Multifunctional Supports of Ultrasmall Pd Nanoparticles for Hydrogenation of Phenol

机译：氮官能化有序介孔碳作为超小钯纳米颗粒对苯酚加氢的多功能载体

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摘要

N-functionalized ordered mesoporous carbons could be readily obtained by post-synthesis treatment with nitrogen containing molecules to achieve materials with a nitrogen loading as high as 8.6 wt % and well preserved mesopore structure. Using NH3 as nitrogen source dramatically ncreased the Brunauer-Emmett-Teller (BET) surface area and pore volume of the resultant hybrid material; however, N- doping with melamine as a source resulted in the contrary results. The N-doped carbons were used as supports to immobilize small-sized Pd nanoparticles (PdNPs), which provided a unique platform to investigate the influence of metal nanoparticle size, mesostructural properties, and N-functionalized supports on the selective hydrogenation of phenol to cyclohexanone, an mportant intermediate in the production of nylon 6 and nylon 66 in the chemical industry. The catalyst with ultrasmall (about 1.2 nm) PdNPs gave the best reaction activity and selectivity under mild conditions. In addition, the present multifunctional catalyst demonstrated excellent catalytic stability and could be used 6 times without loss of product yields. This outstanding catalytic performance could be attributed to the synergetic effects of mesoporous structure, N-functionalized supports, and the stabilized ultrasmall PdNPs. This work might open new avenues for the development of functionalized catalysts with supported ultrasmall metal nanoparticles and hybrid porous support as well as their clean catalyses.
机译：通过用含氮分子进行后合成处理，可以容易地获得N-官能化的有序介孔碳，从而获得具有高达8.6 wt％的氮负载和良好保存的介孔结构的材料。使用NH3作为氮源，极大地增加了所得杂化材料的Brunauer-Emmett-Teller（BET）表面积和孔体积。但是，以三聚氰胺为源进行N掺杂会导致相反的结果。 N掺杂碳用作固定化小型Pd纳米颗粒（PdNP）的载体，这为研究金属纳米颗粒尺寸，介观结构性质和N-官能化载体对苯酚选择性加氢成环己酮的影响提供了独特的平台，是化学工业中尼龙6和尼龙66生产的重要中间体。具有超小（约1.2 nm）PdNP的催化剂在温和条件下具有最佳的反应活性和选择性。另外，本发明的多功能催化剂显示出优异的催化稳定性，并且可以使用6次而不会损失产物收率。这种出色的催化性能可归因于介孔结构，N-官能化载体和稳定的超小PdNP的协同作用。这项工作可能会为功能化催化剂的开发开辟新的途径，该功能化催化剂具有负载的超小金属纳米颗粒和杂化多孔载体以及它们的清洁催化剂。

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