4.8 Article

Designing supported ZnNi catalysts for the removal of oxygen from bio-liquids and aromatics from diesel

Journal

GREEN CHEMISTRY
Volume 14, Issue 10, Pages 2759-2770

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c2gc35901d

Keywords

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Funding

  1. Spanish Secretary of Research, Innovation and Development [CTQ2010-19623, CTQ2006-03008/PPQ, ENE2007-67533-C02-01]
  2. Comunidad de Madrid [S2009ENE-1743]
  3. University of the Basque Country [UFI 11/39]
  4. Basque Government [GIC07/24-IT-220-07]

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This work describes the effect of the support (TiO2, hybrid 2TiO(2)-SiO2, SBA-15 and SBA-15 decorated with TiO2 particles) on the catalytic activity of ZnNi catalysts in the gas-phase hydrodeoxygenation (HDO or O-removal) of phenol and the liquid-phase hydrodearomatization (HDA) of synthetic diesel. These reactions are representative of the two major challenges of the hydrotreating unit embedded in a sustainable refinery: (i) decreasing oxygen content of bio-oils (produced in the pyrolysis of lignocellulosic biomass); and (ii) decreasing aromatics content in diesel. The fresh and deactivated catalysts were characterized by XRD, N-2 adsorption-desorption, TPR, MS/TPD-NH3, XPS, SEM, HRTEM and coke combustion. Under steady-state conditions, the ZnNi catalyst supported on SBA-15 decorated with TiO2 particles displayed the highest activity in the hydrodeoxygenation of phenol (selectivity toward deoxygenated products > 95%) whereas the ZnNi/SBA-15 catalyst displayed the highest activity in the hydrodearomatization of synthetic diesel. It has been shown that dispersion of the active ingredient is favoured on the SBA-15 substrate. The relationship between structure and activity demonstrated that HDO and HDA reactions require optimized metal dispersion and acid function, metal dispersion being more important for HDA than for HDO reactions.

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