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Abstract <p>Catalytic transfer hydrogenation of ethyl levulinate (ELevu) to γ-valerolactone (GVL) is a promising approach to obtaining cyclic ester as a potential solvent and precursor for biofuels from renewable biomass. Herein, a series of ZrO<sub>2</sub> supported on alkali metal-exchanged ZSM-5 (ZrO<sub>2</sub>/MZ-5; M = Li, Na, K and Z-5 = ZSM-5) catalysts is synthesised via a hydrothermal approach, and their catalytic performance is tested for ELevu to GVL. The ZrO<sub>2</sub>/Li-ZSM-5 (ZrO<sub>2</sub>/LZ-5) displays more than five-fold higher catalytic activity in terms of GVL yield than ZrO<sub>2</sub> deposited on parent H-ZSM-5 (ZrO<sub>2</sub>/HZ-5) under identical conditions and affords a maximum yield of 89.9% under optimised reaction conditions. The synthesised ZrO<sub>2</sub>/MZ-5 catalysts are characterised by various techniques, such as X-ray diffraction, N<sub>2</sub>-sorption analysis, NH<sub>3</sub>- and CO<sub>2</sub>-temperature programmed desorption studies, and X-ray photoelectron spectroscopy to understand their structural and surface properties. It is observed that ZrO<sub>2</sub>/LZ-5 possesses a higher number of basic (266 µmol/g) and a lower number of acidic sites (974 µmol/g) compared to ZrO<sub>2</sub>/HZ-5 (193 and 1107 µmol/g). Poisoning studies with 2-nitrobenzoic acid, which passivates basic sites in ZrO<sub>2</sub>/LZ-5, show a significant loss of activity, signifying the pivotal role of basic sites in catalysing Elevu to GVL. The ZrO<sub>2</sub>/LZ-5 catalyst is recyclable with no significant loss of activity in terms of GVL yield for three runs.</p> Graphical Abstract <p></p>

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Synergistic Effect of ZrO2/M-ZSM-5 with Enhanced Basicity for Selective Production of γ-valerolactone from Ethyl Levulinate

  • 期刊论文

  • 发表日期：

    2025年6月24日

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  • Digvijay Badghaiya,
  • Rahul Gautam,
  • Shunmugavel Saravanamurugan,
  • Jigisha K. Parikh,
  • Parimal A. Parikh

摘要

Abstract

Catalytic transfer hydrogenation of ethyl levulinate (ELevu) to γ-valerolactone (GVL) is a promising approach to obtaining cyclic ester as a potential solvent and precursor for biofuels from renewable biomass. Herein, a series of ZrO2 supported on alkali metal-exchanged ZSM-5 (ZrO2/MZ-5; M = Li, Na, K and Z-5 = ZSM-5) catalysts is synthesised via a hydrothermal approach, and their catalytic performance is tested for ELevu to GVL. The ZrO2/Li-ZSM-5 (ZrO2/LZ-5) displays more than five-fold higher catalytic activity in terms of GVL yield than ZrO2 deposited on parent H-ZSM-5 (ZrO2/HZ-5) under identical conditions and affords a maximum yield of 89.9% under optimised reaction conditions. The synthesised ZrO2/MZ-5 catalysts are characterised by various techniques, such as X-ray diffraction, N2-sorption analysis, NH3- and CO2-temperature programmed desorption studies, and X-ray photoelectron spectroscopy to understand their structural and surface properties. It is observed that ZrO2/LZ-5 possesses a higher number of basic (266 µmol/g) and a lower number of acidic sites (974 µmol/g) compared to ZrO2/HZ-5 (193 and 1107 µmol/g). Poisoning studies with 2-nitrobenzoic acid, which passivates basic sites in ZrO2/LZ-5, show a significant loss of activity, signifying the pivotal role of basic sites in catalysing Elevu to GVL. The ZrO2/LZ-5 catalyst is recyclable with no significant loss of activity in terms of GVL yield for three runs.

Graphical Abstract