1. Ru/CeO2 catalyst with optimized CeO2 morphology and surface facet for efficient hydrogenation of ethyl levulinate to γ-valerolactone.
- Author
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Gao, Xiaoqing, Zhu, Shanhui, Dong, Mei, Wang, Jianguo, and Fan, Weibin
- Subjects
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RUTHENIUM catalysts , *SURFACE morphology , *CATALYSTS , *HYDROGENATION , *ACTIVATION energy - Abstract
• Rod, cube and octahedral CeO 2 exposed (1 1 0), (1 0 0) and (1 1 1) facets in Ru/CeO 2. • Ru/CeO 2 -rod with exposed (1 1 0) facet achieved 99.4% GVL yield in EL hydrogenation. • DFT calculation elucidates reaction mechanism of EL hydrogenation to GVL on Ru/CeO 2. • The concentration of oxygen vacancy is linearly proportional to GVL production rate. • Surface CeO 2 structure and concentration of oxygen vacancy determine facet effect. Three Ru/CeO 2 catalysts with different CeO 2 morphology (nanorod, nanocube and nano-octahedra) mainly exposed (1 1 0) + (1 0 0), (1 0 0) and (1 1 1) facets for hydrogenation of biomass-derived ethyl levulinate (EL) to valuable γ-valerolactone (GVL). Ru/CeO 2 -rod with exposed (1 1 0) crystal plane obtained the highest GVL yield (99.4%) and best productivity (13140 h−1). The surface facets of CeO 2 supports not only affect the chemical states of Ru species but also tune the concentration of oxygen vacancy in Ru-CeO 2 interface. The concentration of oxygen vacancy shows a linear relationship with GVL production rate. DFT calculations indicate that the lactonization of CH 3 CHOCH 2 CH 2 CO* to produce GVL is the rate-determining step in EL hydrogenation, and Ru 10 /CeO 2 (1 1 0) with more oxygen vacancy has low activation energy barrier, compared to Ru 10 /CeO 2 (1 0 0) and Ru 10 /CeO 2 (1 1 1). [ABSTRACT FROM AUTHOR]
- Published
- 2020
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