期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 300, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120746
关键词
Bifunctional catalyst; Hydrogenation-dehydration; Lewis acidic sites; Lower energy barrier; Metal-support interaction; Synergistic effect
资金
- National Natural Science Foundation of China, China [21763031, 22062025]
- Yunnan Funda-mental Research Projects, China [202001AW070012,202101AT070171]
- National Special Funds of China, China [C176220100063]
- Program for Excellent Young Talents of Yunnan University, China
- Open Research Fund of School of Chemistry and Chemical Engineering of Henan Normal University, China
The study demonstrates the unique synergy in the SnxMn1Oy oxide, which can enhance the hydrogenation catalysis of Pt nanoparticles for the conversion of LA to GVL. Through a series of Pt/SnxMn1Oy catalysts, it is found that the intrinsic TOF shows a volcano-like dependence on Pt-0 sites and Lewis acidity; the optimal Pt/Sn0.8Mn1Oy catalyst shows high efficiency under specific conditions.
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.
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