1. Yunnan Univ, Natl Demonstrat Ctr Expt Chem & Chem Engn Educ, Sch Chem Sci & Technol, Key Lab Med Chem Nat Resource,Minist Educ, 2 North Cuihu Rd, Kunming 650091, Yunnan, Peoples R China
2. Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China
折叠
Abstract
The synergistic effect in a bimetallic oxide usually plays a vital role in determining the behavior of supported-metal catalysts. We show the unique synergy in a SnxMn1Oy oxide, which can boost the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid (LA) to gamma-valerolactone (GVL). On a series of Pt/SnxMn1Oy catalysts with a similar Pt loading (ca. 0.44 wt%) and a controlled Pt size (ca. 2.7 nm), the intrinsic TOF presents a volcano-like dependence on Pt-0 sites and Lewis acidity, which is determined by the variable synergistic effect between MnOy and SnOy. The optimal Pt/Sn0.8Mn1Oy catalyst exhibits a high iTOF of 2709 h(-1) and achieves 100% selectivity to GVL at 99% conversion of LA at 120 degrees C and 2 MPa of H-2. DFT calculations demonstrate that the incorporation of Sn can provide a lower energy barrier for the crucial elementary reactions.
Key words
Bifunctional catalyst/Hydrogenation-dehydration/Lewis acidic sites/Lower energy barrier/Metal-support interaction/Synergistic effect