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Highly Efficient Transfer Hydrogenation of Levulinate Esters to γ-Valerolactone over Basic Zirconium Carbonate

Author:
Li, Fukun, Li, Zhangmin, France, Liam John, Mu, Jiali, Song, Changhua, Chen, Yuan, Jiang, Lilong, Long, Jinxing, Li, Xuehui
Source:
Industrial & engineering chemistry process design and development 2018 v.57 no.31 pp. 10126-10136
ISSN:
1520-5045
Subject:
biomass, carbonates, catalysts, catalytic activity, esters, hydrogen, hydrogenation, lead, magnesium, nickel, nitrogen, process design, value added, zinc, zirconium
Abstract:
Novel and selective strategies for platform chemical production from renewable biomass are highly attractive in respect to value-added utilization of sustainable resources. In this study, a series of low-cost, commercially available, transition metal carbonates (Zr, Ni, Mg, Zn, and Pb) were investigated for catalytic transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) via the cascade process of Meerwein–Ponndorf–-Verley (MPV) reduction and lactonization reaction. Among the selected catalysts, basic zirconium carbonate is the most active, with the highest turnover frequency (TOF) of 3.1 h–¹ and a surface reaction rate of 0.21 mol m–² h–¹. At 453 K, 3.0 h, and 1.0 MPa N₂, 100% ethyl levulinate conversion, 96.3% GVL yield, and 91.9% hydrogen donor utilization are observed due to the cooperative effect between acid (Mⁿ⁺) and base (−OH) sites. Furthermore, this catalyst shows high recyclability under the optimized conditions, where a satisfactory catalytic activity is shown even after six consecutive runs.
Agid:
6086996