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Catalytic reactivity of an iridium complex with a proton responsive N-donor ligand in CO2 hydrogenation to formate

机译:铱与质子响应性N-供体配体在CO 2 加氢制甲酸反应中的催化反应

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Catalytic hydrogenation of CO2 into formic acid/formate is an attractive conversion in the utilization of CO2. Although various catalysts with high catalytic efficiency are reported, a very few studies have been carried out to correlate/understand the efficacy and stability of the hydrogenation catalysts, which could be helpful to direct the future design strategy of corresponding catalysts. Herein, a half-sandwich iridium complex containing bibenzimidazole as a proton responsive N-donor ligand, [Cp*Ir(BiBzImH2)Cl]Cl, has been synthesized and fully characterized. The generation of an N? anion by the deprotonation of a bibenzimidazole group resulted in a significant enhancement of activity. The Ir complex showed about 20 times higher catalytic efficiency in the hydrogenation of CO2 into formate than that of its bipyridine counterpart [Cp*Ir(Bpy)Cl]Cl. The time dependent catalytic activity studies revealed that the initial excellent activity of [Cp*Ir(BiBzImH2)Cl]Cl was reduced when catalytic cycle proceeds; which was found to be the structural instability of the catalyst caused by steric hindrance between the bibenzimidazole and Cp* ligands.
机译:CO 2 的催化加氢成甲酸/甲酸酯是利用CO 2 的有吸引力的转化方式。尽管已经报道了各种具有高催化效率的催化剂,但是已经进行了很少的研究来关联/理解氢化催化剂的功效和稳定性,这可能有助于指导相应催化剂的未来设计策略。在此,已合成并完全合成了包含联苯并咪唑作为质子响应性N-供体配体[Cp * Ir(BiBzImH 2 )Cl] Cl的半三明治铱络合物。表征。通过联苯并咪唑基团的去质子化反应生成N 阴离子可显着提高活性。 Ir配合物在CO 2 加氢成甲酸中的催化效率比联吡啶对应物[Cp * Ir(Bpy)Cl] Cl高出约20倍。随时间变化的催化活性研究表明,[Cp * Ir(BiBzImH 2 )Cl] Cl的初始优异活性随催化循环的进行而降低。发现这是由于联苯并咪唑和Cp *配体之间的位阻引起的催化剂结构不稳定性。

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