4.8 Article

Selective Hydrodeoxygenation of Lignin-Derived Phenols to Cyclohexanols or Cyclohexanes over Magnetic CoNx@NC Catalysts under Mild Conditions

Journal

ACS CATALYSIS
Volume 6, Issue 11, Pages 7611-7620

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b01785

Keywords

cobalt nitrides; nitrogen-doped carbon; biomass; hydrodeoxygenation; phenols conversion

Funding

  1. NSFC [21572213, 21325208]
  2. National Basic Research Program of China [2012CB215306]
  3. Anhui Provincial Natural Science Foundation [1408085MKL04]
  4. Program for Changjiang Scholars and Innovative Research Team in University of the Ministry of Education of China
  5. Fundamental Research Funds for the Central Universities [wk 2060190040]

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The hydrodeoxygenation (HDO) of lignin derived phenols is important to produce the renewable biofuels. Herein, we reported a simple method to prepare magnetic nitrogen-doped carbon supported cobalt nitride catalysts (CoNx@NC) by copyrolysis of cellulose and cobalt nitrate under ammonia atmosphere. The catalysts were prepared at different temperatures and characterized by elemental analysis, atomic absorption spectroscopy (AAS), Brunauer-Emmett-Teller (BET) surface area analysis, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and temperature-programmed reduction (TPR). The CoNx@NC-650 (pyrolyzed at 650 degrees C) exhibited the best HDO activity for eugenol conversion among a series of Co-based catalysts. The yield of propylcyclohexanol from eugenol was >99.9% under 2 MPa H-2 at 200 degrees C for 2 h. Moreover, a high yield of propylcyclohexane (99.1%) could be achieved when the solid acid HZSM-5 was added to the reaction system. Other lignin-derived phenolic compounds were also investigated and the yield of alkanes was >90%. Based on the mechanism investigation, the catalyst demonstrated a high selectivity to cleave the C-aryl-OR bond under mild conditions.

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