Polydentate pyridyl ligands and the catalytic activity of their iron(II) complexes in oxidation reactions utilizing peroxides as the oxidants
作者:Matthew Lenze、Sergey L. Sedinkin、Eike B. Bauer
DOI:10.1016/j.molcata.2013.03.006
日期:2013.7
activity in that solvent. For the complexes [Fe(10)2](OTf)2 (two tridentate ligands), [Fe(12)(OTf)2] (one tetradentate ligand) and [Fe(16)(OTf)](OTf) (one pentadentate ligand), the product formation for a test reaction was followed over time at significantly reduced catalyst loading to determine activities. Under these conditions, the complex [Fe(10)2](OTf)2 exhibited a somewhat lower catalytic activity
本文介绍了带有新的多齿N,O-配位吡啶基配体的铁(II)配合物的合成及其在以过氧化物为氧化剂的氧化反应中的催化应用。三齿N,O,N(10)和N,N,O(11)配体,四齿N,N,O,N配体12和五齿N,N,N,O,N合成了配位体16,以油或固体的形式得到,分离出的产率为74-93%。随后将配体转化为铁络合物[Fe(10)2 ](OTf)2,[Fe(11)2 ](OTf)2,[Fe(12)(OTf)2 ]和[Fe(16)( OTf)](OTf),以棕褐色粉末的形式获得,收率为90-94%,并通过各种仪器技术进行了表征。初步筛选实验表明,所有络合物在仲醇和苄基亚甲基氧化为相应的酮中均具有催化活性。配合物[Fe(12)(OTf)2 ]产生了一种系统,该系统在温和条件下从苄基亚甲基和仲醇制得的酮的分离产率为63-90%(3摩尔%的催化剂负载量,CH 3 CN中3当量H 2 O 2,反应2 h在室温下