Sanjeev Kushwaha, Tushar A. Kharde, Ralf Köppe and Sanjay Kumar Singh*,
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引用次数: 0
Abstract
Herein, we synthesized water-soluble ruthenium complexes [(η6-p-cymene)Ru(κ2-L)]+ ([C-1]–[C-5]) ligated with substituted bis-imidazole methane-based ligands (L1–L5) and the molecular structures of the representative complexes [C-2] and [C-4] were established by single-crystal X-ray diffraction. We screened the synthesized complexes for the catalytic dehydrogenation of formic acid (FA) in water, where substitution on the bis-imidazole methane ligands was found to exert a significant impact on the catalytic activity of the complexes. The results inferred that, among the screened catalysts, [C-5] outperformed others with an initial turnover frequency (TOF) of 1831 h–1 at 90 °C. One of the most notable features of [C-5] was its exceptional long-term stability, as it maintained efficient H2 production from FA for 35 catalytic runs and remained active even after 60 days without any significant deactivation, reaching a turnover number (TON) of 35,000. Furthermore, reaction kinetics and the influence of various reaction parameters are thoroughly examined; comprehensive mass and NMR investigations under both catalytic and control conditions are conducted, and theoretical studies are performed to gain more insights into the reaction pathway of FA dehydrogenation over the studied catalysts.
期刊介绍:
Organometallics is the flagship journal of organometallic chemistry and records progress in one of the most active fields of science, bridging organic and inorganic chemistry. The journal publishes Articles, Communications, Reviews, and Tutorials (instructional overviews) that depict research on the synthesis, structure, bonding, chemical reactivity, and reaction mechanisms for a variety of applications, including catalyst design and catalytic processes; main-group, transition-metal, and lanthanide and actinide metal chemistry; synthetic aspects of polymer science and materials science; and bioorganometallic chemistry.