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首页> 外文期刊>RSC Advances >New hybrid materials based on the grafting of Pd(ii)-amino complexes on the graphitic surface of AC: preparation, structures and catalytic properties
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New hybrid materials based on the grafting of Pd(ii)-amino complexes on the graphitic surface of AC: preparation, structures and catalytic properties

机译：基于Pd（II）-氨基络合物在AC的石墨表面接枝的新型混合材料：制备，结构和催化性能

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A novel procedure for the preparation of solid Pd( II )-based catalysts consisting of the anchorage of designed Pd( II )-complexes on an activated carbon (AC) surface is reported. Two molecules of the Ar–S–F type (where Ar is a plane-pyrimidine moiety, F a Pd( II )-ligand and S an aliphatic linker) differing in F, were grafted on AC by π–π stacking of the Ar moiety and the graphene planes of the AC, thus favouring the retaining of the metal-complexing ability of F. Adsorption of Pd( II ) by the AC/Ar–S–F hybrids occurs via Pd( II )-complexation by F. After deep characterization, the catalytic activities of the AC/Ar–S–F/Pd( II ) hybrids on the hydrogenation of 1-octene in methanol as a catalytic test were evaluated. 100% conversion to n -octane at T = 323.1 K and P = 15 bar, was obtained with both catalysts and most of Pd( II ) was reduced to Pd(0) nanoparticles, which remained on the AC surface. Reusing the catalysts in three additional cycles reveals that the catalyst bearing the F ligand with a larger Pd-complexing ability showed no loss of activity (100% conversion to n -octane) which is assigned to its larger structural stability. The catalyst with the weaker F ligand underwent a progressive loss of activity (from 100% to 79% in four cycles), due to the constant aggregation of the Pd(0) nanoparticles. Milder conditions, T = 303.1 K and P = 1.5 bar, prevent the aggregation of the Pd(0) nanoparticles in this catalyst allowing the retention of the high catalytic efficiency (100% conversion) in four reaction cycles.
机译：报道了一种制备具有所设计的Pd（II）的锚固的基于固体Pd（II）的催化剂的新方法 - 在活性炭（Ac）表面上进行复杂。 Ar-S-F型的两个分子（其中Ar是平面 - 嘧啶部分，在A的Ac上接枝在Ac上接枝在AC上的Pd（II）--ligand和S aliphatic接头） AC的部分和石墨烯平面，从而有利于将AC / Ar-S-F杂种的Pd（II）的保留络合能力的保持能力通过Pd（II）通过F.以后的方法进行深度表征，评价AC / Ar-S-F / Pd（II）杂交物的催化活性在甲醇中为催化试验的1-辛烯的氢化。用两种催化剂获得100％在T = 323.1k和P = 15巴特的N-辛烷转化，并且将大部分Pd（II）降低至Pd（0）纳米颗粒，其保持在AC表面上。在三个另外的循环中重用催化剂揭示载体具有较大PD络合能力的F配体的催化剂显示出不损失活性（100％转化为N-辛烷），其被分配到其较大的结构稳定性。由于Pd（0）纳米颗粒的恒定聚集，具有较弱的F配体的催化剂进行了逐渐的活性丧失（从四个循环中的100％至79％）。升温条件T = 303.1 k和P = 1.5巴，防止该催化剂中Pd（0）纳米颗粒的聚集，允许在四个反应循环中保留高催化效率（100％转化率）。

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