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Highly active Ru supported on nitrogen and sulfur co-doped porous carbon for hydrogenation of benzoic acid: Synergy of two dopants

•The high activity of Ru/N1.5S1.5C-800 can be attributed to that the synergistic effect of N, S co-doping changes the physical and chemical properties of the catalyst.•The Ru/N1.5S1.5C-800 catalyst exhibits the highest cyclohexane carboxylic acid yield (99.5 %) for the hydrogenation of benzoic acid....

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Published in:Molecular catalysis 2025-02, Vol.572, p.114767, Article 114767
Main Authors: Wang, Yuyao, Wang, Zijian, Zhu, Lina, Chen, Chunhua, Chen, Wenwen, Gao, Yijing, Song, Tongyang, Chen, Xianlang, Li, Rongrong, Lu, Jiqing
Format: Article
Language:English
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Summary:•The high activity of Ru/N1.5S1.5C-800 can be attributed to that the synergistic effect of N, S co-doping changes the physical and chemical properties of the catalyst.•The Ru/N1.5S1.5C-800 catalyst exhibits the highest cyclohexane carboxylic acid yield (99.5 %) for the hydrogenation of benzoic acid.•The Ru/N1.5S1.5C-800 catalyst displayed excellent stability (conversion remains around 80.0 % and selectivity of 100 %) after twelve reactions.•The Ru/N1.5S1.5C-800 catalyst has more active sites and excellent Ru nanoparticles electronic structure are beneficial to benzoic acid adsorption and reaction. In the field of renewable fine chemicals, the selective hydrogenation of biomass-derived benzoic acid (BA) into cyclohexane carboxylic acid (CCA) holds a pivotal position. Herein, a series of nitrogen (N) and sulfur (S) co-doped Ru-based porous carbon catalysts were synthesized using a combination of soft template and impregnation methods and tested for the hydrogenation of BA. The best performance was obtained on a Ru/N1.5S1.5C-800 catalyst, giving a cyclohexane carboxylic acid yield of 99.5 % and a turnover frequency of 609.4 h−1 at 90 °C and 1 MPa. Such good reactivity is related to the synergy of S, N co-doping, which enhances the Ru dispersion and optimizes the electronic structure of Ru nanoparticles for BA adsorption. Furthermore, the Ru/N1.5S1.5C-800 catalyst exhibits good cycling stability. The porous structure, charge transfer, N, S co-doping synergistic effect, catalyst active sites, and catalytic reaction kinetics model were in-depth investigated by experimental and theoretical calculations, therefore, the findings in this work provides an efficient catalyst choice for the catalytic hydrogenation of BA under mild conditions. The prepared Ru/N1.5S1.5C-800 showed excellent catalytic activity and selectivity in the hydrogenation of benzoic acid to cyclohexane carboxylic acid, and it has high stability with cycle at least five times. [Display omitted]
ISSN:2468-8231
2468-8231
DOI:10.1016/j.mcat.2024.114767