Thermoregulated Ionic Liquid-Stabilizing Ru/Coo Nanocomposites For Catalytic Hydrogenation

LANGMUIR(2020)

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摘要
Catalytic hydrogenations represent fundamental processes and allow for atom-efficient and clean functional group transformations for the production of chemical intermediates and fine chemicals in chemical industry. Herein, the Ru/CoO nanocomposites have been constructed and applied as nanocatalysts for the hydrogenation of phenols and furfurals into the corresponding cyclohexanols and tetrahydrofurfuryl alcohols, respectively. The functionalized ionic liquid acted not only as a ligand for stabilizing the Ru/CoO nanocatalyst but also as a thermoregulated agent. The as-obtained nanocatalyst showed superior activity, and it could be conveniently recovered via the thermoregulating phase separation. In six recycle experiments, the catalysts maintained excellent performance. It was observed that the catalytic performance highly hinged on the molar ratio of Ru to Co in the nanocatalyst. The catalyst characterization was carried out by high-resolution transmission electron microscopy (HRTEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy, X-ray diffraction, high-resolution mass spectrometry, Fourier transform infrared, nuclear magnetic resonance, and UV-vis. Especially, the characterization by HRTEM and HAADF-STEM images of the nanocatalyst demonstrated that Ru(0) and Co(II) species were distributed uniformly and the Ru and Co(II) species were close to each other. However, Co(0) was generated and an electronic transfer from Co to Ru species could occur under the hydrogenation conditions. The C-13 NMR characterization indicated further that Co(II) sites were mainly responsible for phenol adsorption. Meanwhile, the adjacent electron-rich Ru(0) sites can promote H-2 dissociation and favor for the sequential hydrogenation.
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