4.8 Article

Synergy in Sn-Mn oxide boosting the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid

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

  1. National Natural Science Foundation of China, China [21763031, 22062025]
  2. Yunnan Funda-mental Research Projects, China [202001AW070012,202101AT070171]
  3. National Special Funds of China, China [C176220100063]
  4. Program for Excellent Young Talents of Yunnan University, China
  5. Open Research Fund of School of Chemistry and Chemical Engineering of Henan Normal University, China

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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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