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Metal–Organic Gels Derived from Iron(III) and Pyridine Ligands: Morphology, Self‐Healing and Catalysis for Ethylene Selective Dimerization
Chemistry - An Asian Journal ( IF 3.5 ) Pub Date : 2019-04-10 , DOI: 10.1002/asia.201900131 Botian Li 1 , Xue Zhou 1 , Xiangyun Liu 1 , Haimu Ye 1 , Ying Zhang 1 , Qiong Zhou 1
Chemistry - An Asian Journal ( IF 3.5 ) Pub Date : 2019-04-10 , DOI: 10.1002/asia.201900131 Botian Li 1 , Xue Zhou 1 , Xiangyun Liu 1 , Haimu Ye 1 , Ying Zhang 1 , Qiong Zhou 1
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Metal‐organic gels showing potential application in catalysis have received much concern. In this work, we designed and synthesized two metal‐organic gels based on coordination between FeIII and pyridine ligands at room temperature. The gels were characterized by X‐ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) to reveal their assembly structures and morphologies, and it was found the metal‐organic gel derived from di‐topic ligand was composed of three‐dimensional network of nanofibers, while the gel derived from tri‐topic ligand was constituted of sponge‐like structure with amorphous phase. Rheological analysis showed the gel consisting of nanofiber networks displayed self‐healing property. The gels were used as catalysts for selective ethylene dimerization, and the optimum catalysis results of the gel with nanofibers reached the maximal catalytic activity of 1.48×105 g/(mol Fe⋅h) with C4 yield more than 90 %, whereas the sponge‐like gel only gave 38 % C4 products at the same condition. The higher dimerization selectivity of the former FeIII gel was attributed to its regular assembly structure and lower steric hindrance of the surface metal sites. Due to its catalytic activity, high selectivity and preparation simplicity, the FeIII gel might be potentially applicable for the preparation of C4 α‐olefins.
中文翻译：
铁（III）和吡啶配体衍生的金属有机凝胶：乙烯选择性二聚的形态，自愈和催化
在催化中显示出潜在应用的金属有机凝胶备受关注。在这项工作中，我们基于Fe III之间的配位关系设计并合成了两种金属有机凝胶和吡啶配体在室温下。通过X射线衍射（XRD），扫描电子显微镜（SEM）和透射电子显微镜（TEM）对凝胶进行表征，以揭示它们的组装结构和形态，发现来自对位配体的金属有机凝胶为由三维三维纤维网络组成，而由三位配体衍生的凝胶则由具有无定形相的海绵状结构组成。流变分析表明，由纳米纤维网络组成的凝胶具有自愈特性。该凝胶用作乙烯选择性二聚的催化剂，具有纳米纤维的凝胶的最佳催化效果达到了 C 4为1.48×10 5 g /（mol Fe·h）的最大催化活性。收率超过90％，而海绵状凝胶在相同条件下仅产生38％的C 4产物。前Fe III凝胶较高的二聚化选择性归因于其规则的组装结构和较低的表面金属位阻。由于其催化活性，高选择性和简单制备的Fe III凝胶可能是潜在地适用于C的制备4 α烯烃。
更新日期：2019-04-10
中文翻译：
铁（III）和吡啶配体衍生的金属有机凝胶：乙烯选择性二聚的形态，自愈和催化
在催化中显示出潜在应用的金属有机凝胶备受关注。在这项工作中，我们基于Fe III之间的配位关系设计并合成了两种金属有机凝胶和吡啶配体在室温下。通过X射线衍射（XRD），扫描电子显微镜（SEM）和透射电子显微镜（TEM）对凝胶进行表征，以揭示它们的组装结构和形态，发现来自对位配体的金属有机凝胶为由三维三维纤维网络组成，而由三位配体衍生的凝胶则由具有无定形相的海绵状结构组成。流变分析表明，由纳米纤维网络组成的凝胶具有自愈特性。该凝胶用作乙烯选择性二聚的催化剂，具有纳米纤维的凝胶的最佳催化效果达到了 C 4为1.48×10 5 g /（mol Fe·h）的最大催化活性。收率超过90％，而海绵状凝胶在相同条件下仅产生38％的C 4产物。前Fe III凝胶较高的二聚化选择性归因于其规则的组装结构和较低的表面金属位阻。由于其催化活性，高选择性和简单制备的Fe III凝胶可能是潜在地适用于C的制备4 α烯烃。
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