Supramolecular assembling of molecular ion-ligands on graphite-based solid materials directed to specific binding of metal ions
Supramolecular assembling of molecular ion-ligands on graphite-based solid materials directed to specific binding of metal ions
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DOI：
10.1016/j.ica.2014.02.015
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发表时间：
2014-06-01
影响因子：
2.8
通讯作者：
Javier Lopez-Garzon, F.
中科院分区：
文献类型：
--
作者：
Lopez-Garzon, Rafael;Luz Godino-Salido, M.;Javier Lopez-Garzon, F.
具有特殊拓扑结构的分子配体，基于连接到亲水性(金属络合)取代基的极性杂芳核，由于平面型嘧啶部分与AC表面的芳烃中心之间强烈的pi-pi相互作用，与活性碳(AC)形成非常稳定的组装。AC石墨片边缘的杂原子功能不会改变与配体的相互作用模式，也不会改变组装的稳定性。这导致了稳定的杂化产物AC/配体的形成，其表面化学性质，特别是酸碱行为和对金属离子的亲和力，反映了配体的非共轭亲水部分的性质。因此，这种杂化材料表现出比母体AC更好的金属离子吸附能力，并与非共轭取代基的金属结合能力相关。为了有效地将配体非共轭取代基的化学性质转移到杂化AC/配体中，母体AC中需要大量的中孔和大孔。在吸附金属离子后，出现了AC/配体/金属杂化材料，具有有趣的潜在应用。因此，AC/三胺配体/Pd(II)杂化催化剂在加氢反应中表现出很高的催化活性，因为在第一个反应周期中，AC表面形成了高度稳定的Pd纳米颗粒。(C)爱思唯尔出版的2014年。
Molecular ligands with a particular topology, based on a polar heteroaromatic nucleus linked to hydrophilic (metal-complexing) substituents, form very stable assemblies with activated carbons (ACs) due to strong pi-pi interactions between the planar pyrimidine moiety and the arene centers of the AC surfaces. Heteroatomic functions at the edges of the AC graphitic sheets do not alter the interaction mode with the ligands nor the stability of the assemblies. That results in the formation of stable hybrids, AC/ligand, whose surface chemical properties, specially the acid base behavior and the affinity to metal ions, reflect those of the non-conjugated, hydrophilic moieties of the ligands. Consequently, such hybrid materials show metal ion adsorptivities that are superior to those of the parent AC and correlate with the metal-binding abilities of the non-conjugated substituents. Significant amounts of meso-and macropores are required in the parent AC to efficiently transfer the chemical properties of the ligand non-conjugated substituents to the hybrid AC/ligand. After adsorption of metal ions, new hybrids, AC/ligand/metal, emerge with interesting potential applications. Thus, an AC/triamine ligand/Pd(II) hybrid showed high catalytic activity in hydrogenation reactions due to the formation of highly stable Pd nanoparticles at the AC surface during the first reaction cycle. (C) 2014 Published by Elsevier B.V.