Ambient-condition hydrogenation of renewable levulinic acid to γ-valerolactone over metallic-acidic RuPt/MIL-101 catalyst
γ-Valerolactone (GVL) as an important high-value chemical can be readily produced through the catalytic hydrogenation of renewable levulinic acid (LA). However, high reaction temperatures (70–240 ℃) and H 2 pressures (0.5–6 MPa) are usually required to achieve full LA conversion and desired GVL yield in previous studies. Herein, we report, for the first time, the ambient-condition upgrading of LA to GVL by rationally constructing a series of metallic–acidic Ru x Pt y /MIL-101 catalysts comprising RuPt-alloyed nanoparticles (NPs) and Lewis-acid sites within a chromium-based MOF (namely MIL-101). Benefiting from the favorable synergy between Ru and Pt in their alloyed NPs and abundant Lewis-acid sites in MIL-101, the best Ru 4 Pt 1 /MIL-101 featuring an optimized Ru/Pt molar ratio of 4:1 shows a complete LA conversion with > 99.9 % yield of GVL under unprecedented ambient temperature and pressure, affording a high turnover frequency (TOF) of 1480.5h −1 , which is 15.1 and 10.1 times that of its monometallic Pt/MIL-101 (98.3 h −1 ) and Ru/MIL-101 (146.7 h −1 ) counterparts, respectively. Detailed experiments and density functional theory (DFT) calculations suggest the RuPt-alloyed effect and Lewis-acid sites in Ru 4 Pt 1 /MIL-101 can optimize the adsorption energy of 4-hydroxyvaleric acid (HPA) to remarkably boosting its catalytic performance for this reaction.
危险品化学品经营许可证（带存储）