Selectivity

Geology

Organic chemistry

Hydrodesulfurization

Photocatalysis

Biomass (ecology)

Oceanography

Catalysis

Chemistry

Hydrodeoxygenation

Deoxygenation

Hydrodenitrogenation

Graphitic carbon nitride

Mesoporous material

Journal of the American Chemical Society

Hydrogenation and hydrodeoxygenation are significant and distinct approaches for the conversion of biomass and biomass-derived oxygenated chemicals into high value-added chemicals and fuels. However, it remains a great challenge to synthesize catalysts that simultaneously possess excellent hydrogenation and hydrodeoxygenation performance. Herein, we report a catalyst made of isolated single-atom Ru supported on mesoporous graphitic carbon nitride (Ru1/mpg-C3N4), fabricated by a wet impregnation method. The as-prepared Ru1/mpg-C3N4 catalyst shows excellent hydrogenation and hydrodeoxygenation performance. First-principles calculations reveal that the Ru atom is mobilized, and the active site is induced by adsorption of the reactants. A systematic reaction mechanism is proposed, suggesting that vanillyl alcohol is the deoxygenation prohibited product, while 2-methoxy-p-cresol is the deoxygenation allowed product. Thus, the excellent selectivity for the hydrogenation or hydrodeoxygenation of vanillin at different temperatures results from switching between the two types of products.

Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru1/mpg-C3N4 Catalyst