期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 7, 期 19, 页码 16501-16510出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b03742
关键词
Ruthenium nanoparticle; Electronic state; Levulinic acid; Hydrogenation; Biomass
资金
- National Natural Science Foundation of China [21676100]
- Guangdong Natural Science Foundation [2017A030312005]
- Science and Technology Program of Guangzhou City [201707010058]
Ru has been found to be a highly efficient catalyst for producing gamma-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 Ru-0 with lower binding energy (Ru 3p) showed higher activity independent of the parameters of synthesis. Theoretical calculations indicated that the electron-rich Ru-0 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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