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

被引:35
|
作者
Boosa, Venu [1 ]
Varimalla, Shirisha [1 ,2 ]
Dumpalapally, Mahesh [1 ,2 ]
Gutta, Naresh [1 ]
Velisoju, Vijay Kumar [1 ]
Nama, Narender [1 ]
Akula, Venugopal [1 ,2 ]
机构
[1] CSIR Indian Inst Chem Technol, Catalysis & Fine Chem Div, Hyderabad 500007, Telangana, India
[2] Acad Sci & Innovat Res AcSIR, Ghaziabad 201002, India
关键词
Reductive amination; Pyrrolidones; Acetone-pyridine-IR; Cu; H-ZSM-5; N2O titration; LEVULINIC ACID; REDUCTIVE AMINATION; ACTIVE-SITES; GAMMA-VALEROLACTONE; EXCHANGED ZSM-5; SURFACE-ACIDITY; PYRIDINE BASES; BETA ZEOLITES; CU IONS; CONVERSION;
D O I
10.1016/j.apcatb.2021.120177
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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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页数:14
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