期刊
SMALL
卷 14, 期 36, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201801953
关键词
carbothermal; copper; hydrodeoxygenation; transfer-hydrogenation; vanillin
类别
资金
- National Natural Science Foundation of China [51432009, 51502297, 51372248]
- Instrument Developing Project of the Chinese Academy of Sciences [yz201421]
Highly dispersed copper nanoparticles (Cu NPs) supported on activated carbon (AC) are effectively synthesized by one-pot carbothermal method at temperature range of 400-700 degrees C. The X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and Brunauer-Emmett-Teller analysis reveal that Cu NPs with diameters of 20-30 nm are evenly anchored in carbon matrix. The 15 wt%-Cu/AC-600 catalyst (derived at 600 degrees C) exhibits best bifunctional catalysis of aqueous-phase hydrodeoxygenation (HDO) and organic-phase transfer-hydrogenation reaction (THR) to selectively transform vanillin to 2-methoxy-4-methylphenol (MMP). In HDO of vanillin, the as-prepared catalyst achieves a 99.9% vanillin conversion and 93.2% MMP selectivity under 120 degrees C, 2.0 MPa H-2 within 5 h. Meanwhile, near-quantitative vanillin conversion and 99.1% MMP selectivity are also obtained under 180 degrees C within 5 h in THR of vanillin by using 2-propanol as hydrogen donor. The transforming pathways of vanillin are also proposed: vanillin is transformed into MMP via intermediate of 4-hydroxymethyl-2-methoxyphenol in HDO case and by direct hydrogenolysis of vanillin in THR course. More importantly, the activity and the selectivity do not change after 5 cycles, indicating the catalyst has excellent stability. The Cu-based catalyst is relatively cheap and preparation method is facile, green, and easy scale-up, thus achieving a low-cost transformation of biomass to bio-oils and chemicals.
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