摘要
Formic acid(FA)dehydrogenation was investigated over several arene-ruthenium catalysts with various imidazolyl-,thiophenyl-and furyl-based ligands.The catalyst with an N-((1H-imidazol-2-yl)methyl)propan-2-amine ligand(Ru/L7)outperformed other catalysts in FA dehydrogenation at 90℃ in water.Furthermore,the developed process was scaled up by a factor of 10 without any loss in activity.Remarkably,Ru/L7 exhibited high robustness and long-term durability during reusability over 79 catalytic runs,achieving very high turnovers per Ru,releasing 37.6 L of gas(H_(2) and CO_(2))with a productivity rate of 15660 L(H_(2)+CO_(2))molRu−1 h^(−1)(∼7 gH_(2) gRu^(−1) h^(−1)).Advantageously,the Ru/L7 catalyst also promoted CO_(2)hydrogenation to formate at 80℃.Mechanistic insights were gained through KIE studies and via the identification of several catalytic intermediates involved in various steps of catalytic FA dehydrogenation and CO_(2)hydrogenation under catalytic and controlled reaction conditions.
基金
the financial support from IIT Indore,CSIR(01(3045)/21/EMR-II)
DST(CRG/2021/000504).
