Temperature-Controlled Selectivity of Hydrogenation and Hydrodeoxygenation in the Conversion of Biomass Molecule by the Ru1 /mpg-C3 N4 Catalyst

Journal of the American Chemical Society
Shubo TianYadong Li

Abstract

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.

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Citations

Nov 15, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Chun ChenHuijun Zhao
Jul 3, 2019·Advanced Materials·Yuanwen ZhangZiqi Sun
Mar 13, 2020·Advanced Materials·Chao LuXi Chen
Jun 20, 2020·Chemical Communications : Chem Comm·Chenliang YeYadong Li
Nov 16, 2019·Advanced Science·Bin ZhangHan Zhang
Apr 28, 2021·Chemical Society Reviews·Yanan ShangXiaoguang Duan
Apr 4, 2020·Chemical Reviews·Shufang JiYadong Li
Oct 22, 2021·Chemistry : a European Journal·Mahnaz NajafiMehrorang Ghaedi

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