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Ru(III) single site solid micellar catalyst for selective aqueous phase hydrogenation of carbonyl groups in biomass-derived compounds

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Abstract
Catalytic processes in water have a lower environmental impact, cost, and toxicity than in organic solvents. Considering the high content of water in biomass, it would be natural to use aqueous phase catalytic technology for the production of valuable products. However, in the aqueous phase, most metal-based catalysts suffer from low activity, low selectivity and deactivation due to metal oxidation and leaching. In this paper, we propose a solid micellar Ru catalyst (Ru(III)@MCM) based on single-site Ru(III) species stabilized by cetyltrimethylammonium (CTA+) surfactant and immobilized in the walls of MCM-41 for the selective aqueous phase hydrogenation of carbonyl groups. This catalyst demonstrates exceptional selectivity, activity, and stability in comparison with conventional metallic catalysts. DFT modeling suggests that the reaction proceeds via heterolytic dissociation of hydrogen, forming a Ru-Hydride species, and subsequent hydride transfer to the carbonyl group. Water plays a key role in avoiding product inhibition.
Keywords
Process Chemistry and Technology, General Environmental Science, Catalysis, Solid micelles, Ru (III), HydrogenationBiomass, Aqueous phase

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MLA
Wang, Qiyan, et al. “Ru(III) Single Site Solid Micellar Catalyst for Selective Aqueous Phase Hydrogenation of Carbonyl Groups in Biomass-Derived Compounds.” APPLIED CATALYSIS B-ENVIRONMENTAL, vol. 300, 2022, doi:10.1016/j.apcatb.2021.120730.
APA
Wang, Q., Oliveira Santos, S., Urbina-Blanco, C. A., Zhou, W., Yang, Y., Marinova, M., … Ordomsky, V. V. (2022). Ru(III) single site solid micellar catalyst for selective aqueous phase hydrogenation of carbonyl groups in biomass-derived compounds. APPLIED CATALYSIS B-ENVIRONMENTAL, 300. https://doi.org/10.1016/j.apcatb.2021.120730
Chicago author-date
Wang, Qiyan, Sara Oliveira Santos, César A. Urbina-Blanco, Wenjuan Zhou, Yong Yang, Maya Marinova, Svetlana Heyte, et al. 2022. “Ru(III) Single Site Solid Micellar Catalyst for Selective Aqueous Phase Hydrogenation of Carbonyl Groups in Biomass-Derived Compounds.” APPLIED CATALYSIS B-ENVIRONMENTAL 300. https://doi.org/10.1016/j.apcatb.2021.120730.
Chicago author-date (all authors)
Wang, Qiyan, Sara Oliveira Santos, César A. Urbina-Blanco, Wenjuan Zhou, Yong Yang, Maya Marinova, Svetlana Heyte, Thuriot-Roukos Joelle, Ovidiu Ersen, Walid Baaziz, Olga V. Safonova, Mark Saeys, and Vitaly V. Ordomsky. 2022. “Ru(III) Single Site Solid Micellar Catalyst for Selective Aqueous Phase Hydrogenation of Carbonyl Groups in Biomass-Derived Compounds.” APPLIED CATALYSIS B-ENVIRONMENTAL 300. doi:10.1016/j.apcatb.2021.120730.
Vancouver
1.
Wang Q, Oliveira Santos S, Urbina-Blanco CA, Zhou W, Yang Y, Marinova M, et al. Ru(III) single site solid micellar catalyst for selective aqueous phase hydrogenation of carbonyl groups in biomass-derived compounds. APPLIED CATALYSIS B-ENVIRONMENTAL. 2022;300.
IEEE
[1]
Q. Wang et al., “Ru(III) single site solid micellar catalyst for selective aqueous phase hydrogenation of carbonyl groups in biomass-derived compounds,” APPLIED CATALYSIS B-ENVIRONMENTAL, vol. 300, 2022.
@article{8729823,
  abstract     = {{Catalytic processes in water have a lower environmental impact, cost, and toxicity than in organic solvents. Considering the high content of water in biomass, it would be natural to use aqueous phase catalytic technology for the production of valuable products. However, in the aqueous phase, most metal-based catalysts suffer from low activity, low selectivity and deactivation due to metal oxidation and leaching. In this paper, we propose a solid micellar Ru catalyst (Ru(III)@MCM) based on single-site Ru(III) species stabilized by cetyltrimethylammonium (CTA+) surfactant and immobilized in the walls of MCM-41 for the selective aqueous phase hydrogenation of carbonyl groups. This catalyst demonstrates exceptional selectivity, activity, and stability in comparison with conventional metallic catalysts. DFT modeling suggests that the reaction proceeds via heterolytic dissociation of hydrogen, forming a Ru-Hydride species, and subsequent hydride transfer to the carbonyl group. Water plays a key role in avoiding product inhibition.}},
  articleno    = {{120730}},
  author       = {{Wang, Qiyan and Oliveira Santos, Sara and Urbina-Blanco, César A. and Zhou, Wenjuan and Yang, Yong and Marinova, Maya and Heyte, Svetlana and Joelle, Thuriot-Roukos and Ersen, Ovidiu and Baaziz, Walid and Safonova, Olga V. and Saeys, Mark and Ordomsky, Vitaly V.}},
  issn         = {{0926-3373}},
  journal      = {{APPLIED CATALYSIS B-ENVIRONMENTAL}},
  keywords     = {{Process Chemistry and Technology,General Environmental Science,Catalysis,Solid micelles,Ru (III),HydrogenationBiomass,Aqueous phase}},
  language     = {{eng}},
  pages        = {{10}},
  title        = {{Ru(III) single site solid micellar catalyst for selective aqueous phase hydrogenation of carbonyl groups in biomass-derived compounds}},
  url          = {{http://doi.org/10.1016/j.apcatb.2021.120730}},
  volume       = {{300}},
  year         = {{2022}},
}

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