4.8 Article

Influence of Bronsted acid sites on chemoselective synthesis of pyrrolidones over H-ZSM-5 supported copper catalyst

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 292, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.apcatb.2021.120177

关键词

Reductive amination; Pyrrolidones; Acetone-pyridine-IR; Cu; H-ZSM-5; N2O titration

资金

  1. DST, New Delhi under India-Poland program [DST/INT/Pol/P31/2016]

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Cu(0)/H-ZSM-5 was identified as a chemoselective catalyst for the synthesis of pyrrolidones through reductive amination of levulinic acid in aqueous media at ambient pressure. The chemoselective nature of Cu was explained by interactions with surface Bronsted acid sites observed through infrared spectroscopic studies. Decrease in Si/Al ratio of the H-ZSM-5 resulted in increased reductive amination activity, with physicochemical characteristics of the catalysts analyzed by various methods to establish a structure-activity relationship.
Cu(0)/H-ZSM-5 was identified as a chemoselective catalyst in the reductive amination of levulinic acid for the synthesis of pyrrolidones at ambient pressure and in aqueous media. The chemoselective nature of Cu was explained by carbonyl interaction with surface Bronsted acid sites deduced by pyridine and acetone adsorbed in situ infrared (IR) spectroscopic studies in conjunction with N2O titration. A strong polarization of band at 1685 cm-1 and an increase in its intensity with a decrease in Si/Al ratio of the H-ZSM-5 was found to be a key factor in the reductive amination activity. Structure activity relationship was established using the physicochemical characteristics of the catalysts analyzed by XRD, BET-SA, H2-TPR, NH3-TPD and XPS analyses.

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