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

机译:铱络合物的催化反应性与质子响应N-供体配体在CO 2氢化中甲酸甲酸

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摘要

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(BiBzImH(2)) 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的催化氢化成甲酸/甲酸盐是在使用CO 2的利用中具有吸引力的转化。尽管报道了具有高催化效率的各种催化剂,但已经进行了很少的研究以相关/了解氢化催化剂的功效和稳定性,这有助于引导相应催化剂的未来设计策略。这里,已经合成并完全表征了含有Bibenzimidazole的半夹心铱络合物作为质子响应N-供体配体,[CP * IR(BibzimH(2))Cl] Cl。通过甲基密封咪唑基团的去质子化产生n-阴离子导致活性的显着增强。 IR络合物在CO 2的氢化成甲酸盐中显示出约20倍催化效率的催化效率高于其Bi吡啶对应物[CP * IR(BPE)Cl] Cl的甲酸。时间依赖性催化活性研究表明,当催化循环进行时,减少了[Cp * Ir(BibzimH2)Cl] Cl的初始优异活性;被发现是由Bibenzimidazole和CP *配体之间的空间障碍引起的催化剂的结构不稳定性。

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  • 来源
    《RSC Advances》 |2018年第3期|共5页
  • 作者单位

    Kookmin Univ Dept Appl Chem 77 Jeongneung Ro Seoul 136702 South Korea;

    Kookmin Univ Dept Appl Chem 77 Jeongneung Ro Seoul 136702 South Korea;

    Korea Inst Energy Res 152 Gajeong Ro Daejeon 305343 South Korea;

    Kookmin Univ Dept Appl Chem 77 Jeongneung Ro Seoul 136702 South Korea;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
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