Highly Efficient Transfer Hydrogenation of Levulinate Esters to γ‑Valerolactone over Basic Zirconium Carbonate
journal contributionposted on 04.07.2018, 00:00 authored by Fukun Li, Zhangmin Li, Liam John France, Jiali Mu, Changhua Song, Yuan Chen, Lilong Jiang, Jinxing Long, Xuehui Li
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.
Read the peer-reviewed publication
turnover frequencybiomasethylγ- valerolactoneBasic Zirconium Carbonate Novel3.0 hmolresourceOHsurface reaction rateEfficient Transfer HydrogenationseriesPb3.1acidMeerwein0.21transition metal carbonatesMgZnMPVoptimized conditionsrecyclabilityZrNiplatform chemical productionlactonization reactionutilizationtransfer hydrogenationstrategyM nValerolactonecatalystsiteTOFLevulinate Esters1.0 MPa N 2cascade processdonorzirconium carbonateGVLconversionlevulinate esters453 K