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Electron-Rich Ruthenium on Nitrogen-Doped Carbons Promoting Levulinic Acid Hydrogenation to γ‑Valerolactone: Effect of Metal–Support Interaction

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posted on 2019-09-18, 19:44 authored by Zhen Meng, Yong Liu, Guangxing Yang, Yonghai Cao, Hongjuan Wang, Feng Peng, Pengfei Liu, Hao Yu
Ru has been found to be a highly efficient catalyst for producing γ-valerolactone from the hydrogenation of levulinic acid. However, the active species on Ru nanoparticles (NPs) are still unclear. Here, we synthesized a series of Ru NPs with tunable chemical states obtained by altering the interaction with carbon-nanotube-based supports, achieved by the strategies of doping carbon nanotubes with N and S atoms, changing the amount of dopants, and varying the loading of Ru. The surface species of the supported Ru NPs, identified by X-ray photoelectron spectroscopy, were linked to the catalytic activities instrinsically. We found that the Ru NPs possessing Ru0 with lower binding energy (Ru 3p) showed higher activity independent of the parameters of synthesis. Theoretical calculations indicated that the electron-rich Ru0 enhanced LA hydrogenation through facilitating R–COOH breaking into R–CO and −OH, suggesting a powerful tool modifying the catalytic activity of carbon-supported metals by manipulating the electronic metal–support interaction.

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