Key Laboratory of Organic Synthesis of Jiangsu Province, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, People's Republic of China.
Inorg Chem. 2012 Sep 17;51(18):9705-13. doi: 10.1021/ic300949y. Epub 2012 Aug 24.
An efficient strategy for the synthesis of a wide variety of coordination complexes has been developed. The synthetic protocol involves a solvothermal in situ metal-ligand reaction of picolinaldehyde, ammonium acetate, and transition-metal ions, leading to the generation of 12 coordination complexes supported by a novel class of substituted 1-pyridineimidazo[1,5-a]pyridine ligands (L1-L5). The ligands L1-L5 were afforded by metal-mediated controllable conversion of the aldehyde group of picolialdehyde into a ketone and secondary, tertiary, and quaternary carbon centers, respectively. Complexes of various nuclearities were obtained: from mono-, di-, and tetranuclear to 1D chain polymers. The structures of the in situ formed complexes could be controlled rationally via the choice of appropriate starting materials and tuning of the ratio of the starting materials. The plausible mechanisms for the formation of the ligands L1-L5 were proposed.
已经开发出一种有效合成各种配位化合物的策略。该合成方案涉及在溶剂热条件下进行吡啶甲醛、醋酸铵和过渡金属离子的原位金属-配体反应，从而生成由新型取代 1-吡啶基咪唑并[1,5-a]吡啶配体（L1-L5）支持的 12 个配位化合物。配体 L1-L5 通过金属介导的对吡啶甲醛醛基的可控转化为酮基和仲、叔和季碳原子中心分别得到。得到了各种核数的配合物：从单核、双核和四核到 1D 链聚合物。通过选择合适的起始材料和调节起始材料的比例，可以合理控制原位形成的配合物的结构。提出了形成配体 L1-L5 的可能机制。
