Journal
GREEN CHEMISTRY
Volume 23, Issue 13, Pages 4673-4684Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0gc04377j
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Funding
- Australian Research Council
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The study demonstrates that Ni/BEA and Ni/MOR catalysts show better performance in the hydrogenation of toluene, while Ni/BEA is more effective in the hydrodeoxygenation of anisole.
Natural and synthetic (BEA, MOR) zeolite-supported nickel (similar to 5 wt%) catalysts were prepared and employed for the hydrogenation of toluene and hydrodeoxygenation of anisole in a continuous-flow reactor. Ni/BEA and Ni/MOR display a higher level of metal dispersion and stronger metal-support interaction compared to the Ni/NZ and Ni/Escott catalysts, resulting in a higher concentration of charge-compensating Ni species and a larger high-temperature reduction peak. The Ni/BEA and Ni/MOR also present a significant mass of low-temperature desorbed H-2 (centred at 150 degrees C) based on H-2-TPD, suggesting the H species are weakly adsorbed on small Ni clusters. In contrast, the H species were strongly adsorbed by the bulk Ni crystal over Ni/Escott and Ni/NZ, which were desorbed at maxima between 211 and 222 degrees C. We propose that the strongly adsorbed H species play a crucial role in the hydrogenation of toluene, leading to a significantly higher yield of methylcyclohexane over Ni/Escott and Ni/NZ compared to Ni/BEA and Ni/MOR. Both metal and acid sites are required in the hydrodeoxygenation of anisole. The strong Bronsted acid sites and numerous smaller Ni species over Ni/BEA facilitated the transalkylation of anisole to phenol and methylanisole and subsequently hydrogenolysis of phenol to benzene, followed by the hydrogenation of benzene to cyclohexane.
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