Polyethylene Glycol–Bridged Diimidazolium Polyoxometalates: Thermoregulated Reusable Catalysts for Selective Oxidation of Toluene to Benzaldehyde

IF 3.7 2区化学 Q2 CHEMISTRY, APPLIED

Applied Organometallic Chemistry Pub Date : 2024-12-10 DOI:10.1002/aoc.7935

Shu Qian, Fengli Yu, Yexin Luo, Bing Yuan, Congxia Xie, Shitao Yu

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Abstract

The oxidation of toluene to benzaldehyde holds great industrial significance, and it typically involves toxic reagents and/or affords difficult-to-separate product mixtures. Herein, polyethylene glycol (PEG)–bridged diimidazolium polyoxometalates (POMs) with a Keggin-type tungstovanadophosphoric heteropolyacid anion and various PEG-functionalized diimidazolium cations were prepared and evaluated as catalysts for the eco-friendly oxidation of toluene using aqueous tert-butyl hydroperoxide in acetonitrile. The bridging of diimidazolium cations by PEG enabled the fine-tuning of heteropolyanion redox properties and increased catalyst reactivity and solubility in the reaction system. The best-performing POM exhibited thermoregulated phase-separation behavior, that is, it was fully soluble in the reaction medium at elevated temperatures and hardly soluble at room temperature. Further, it showed almost no performance deterioration after sevenfold reuse and achieved an acceptable toluene conversion (82%) and benzaldehyde selectivity (68%). Thus, our work enables the development of eco-friendly processes for the catalytic oxidation of industrially relevant hydrocarbon and thus facilitates the establishment of a more sustainable society.

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来源期刊

Applied Organometallic Chemistry 化学-无机化学与核化学

CiteScore

7.80

自引率

10.30%

发文量

408

审稿时长

2.2 months

期刊介绍： All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.