Simakova IL, Demidova YS, Gläsel J, Murzina EV, Schubert T, Prosvirin IP, Etzold BJ, Murzin DY (2016)
Publication Language: English
Publication Type: Journal article
Publication year: 2016
Book Volume: 6
Pages Range: 8490-8504
Journal Issue: 24
DOI: 10.1039/C6CY02086K
Polyvinylpyrrolidone (PVP) stabilized Ru nanoparticles (NPs) with the mean size ca. 2.4 nm were synthesized and immobilized on mesoporous Sibunit, macroporous carbon nanofibers of platelet structure (CNF-Pl) and micro-/mesoporous TiC carbide-derived carbon (CDC) providing 1.7-2.9 wt.% Ru/C catalysts with the mean Ru size 2.1-2.7 nm. The presence of PVP on the catalyst surface drastically diminished activity in structure sensitive galactose to galactitol hydrogenation. Different PVP removal and support modification methods were tested to elucidate the effect of support hydrophilicity/ hydrophobicity, preliminary support functionalization, additional Ru NPs washing prior to immobilization as well as PVP removal degree on catalytic behavior. For characterization of the carbon supports and synthesized catalysts TEM, XPS, XRD, XRF, water adsorption/desorption experiments and N2 physisorption were applied. Carbon supports were functionalized before Ru NPs immobilization by treatment with 5 wt.% HNO3, HNO3 conc., Ar (700oC), air (350oC), H2 (700oC) without visible support microstructure alterations. Several protocols for PVP removal were applied such as solvothermal (with water and acetic acid aqueous solutions at 220°C) and thermal treatment (in air, argon, hydrogen or nitrogen at different temperatures) not resulting in noticeable changes in Ru NPs size. The thermal treatment in air at 180°C followed by reduction at 250°C was found to be more effective in the case of Sibunit and CNF-Pl while solvothermal treatment in water at 220°C (PN2 25 bar) improved significantly the activity of TiC-CDC based catalysts. Untreated Sibunit and CNF-Pl carbon supports provided higher activity in galactose hydrogenation with Ru/Sibunit exhibiting the best catalytic activity being also the most hydrophilic according to water sorption isotherms. Catalytic activity of untreated micro-/mesoporous Ru/TiC-CDC increased noticeably depending on the support pretreatment in the row: untreated < 5% HNO3 < HNO3 conc. Additional TiC-CDC support functionalization was proposed to be required because of a relatively low amount of oxygen-containing groups on the surface compared to Sibunit and CNF.
APA:
Simakova, I.L., Demidova, Y.S., Gläsel, J., Murzina, E.V., Schubert, T., Prosvirin, I.P.,... Murzin, D.Y. (2016). Controlled synthesis of PVP-based carbon supported Ru nanoparticles: Synthesis approaches, characterization, capping agent removal and catalytic behavior. Catalysis: Science and Technology, 6(24), 8490-8504. https://doi.org/10.1039/C6CY02086K
MLA:
Simakova, I. L., et al. "Controlled synthesis of PVP-based carbon supported Ru nanoparticles: Synthesis approaches, characterization, capping agent removal and catalytic behavior." Catalysis: Science and Technology 6.24 (2016): 8490-8504.
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