Journal of Organometallic Chemistry ( IF 2.3 ) Pub Date : 2020-11-27 , DOI: 10.1016/j.jorganchem.2020.121631 Anshu Singh , Ankur Maji , Aurobinda Mohanty , Kaushik Ghosh
A new family of base-metal nickel complexes [Ni(L1-10)2] (1-10) were synthesized from tridentate meridional ligands L1H to L10H (where H stands for dissociable proton). Different spectroscopic studies were utilized for the characterization of these complexes [Ni(L1-10)2] (1-10). Molecular structures of complexes [Ni(L1)2] (1), [Ni(L3)2] (3) and [Ni(L8)2] (8) were determined by X-ray crystallography. Electronic properties of complexes [Ni(L1)2] (1) [Ni(L3)2] (3) and [Ni(L8)2] (8) were elucidated with the help of DFT and TD-DFT calculations. Complexes [Ni(L1-10)2] (1-10) were utilized as catalysts for the synthesis of 1-butene from ethylene using diethyl aluminium chloride as a co-catalyst. A nearly selective formation of 1-butene was observed and productivity up to 17.50 [kg (product/gm catalyst)] h−1 bar−1 was found after examining the catalytic activity of complexes 1-10. A reaction pathway was also proposed for the conversion of ethylene to 1-butene.
中文翻译:
贱金属镍(II)基催化剂的设计与合成:由乙烯几乎选择性形成1-丁烯的研究
从三齿子午线配体L 1 H到L 10 H(其中H代表可解离的质子)合成了新的贱金属镍配合物[Ni(L 1-10)2 ](1-10)系列。不同的光谱学研究用于表征这些配合物[Ni(L 1-10)2 ](1-10)。配合物[Ni(L 1)2 ](1),[Ni(L 3)2 ](3)和[Ni(L 8)2 ](8)的分子结构通过X射线晶体学测定。借助DFT和TD-DFT计算阐明了配合物[Ni(L 1)2 ](1)[Ni(L 3)2 ](3)和[Ni(L 8)2 ](8)的电子性质。使用配合物[Ni(L 1-10)2 ](1-10)作为催化剂,使用二乙基氯化铝作为助催化剂由乙烯合成1-丁烯。观察到几乎选择性地形成了1-丁烯,生产率高达17.50 [kg(产品/ gm催化剂)] h -1 bar -1在检查了配合物1-10的催化活性后发现。还提出了用于乙烯转化为1-丁烯的反应途径。