(247f) Silica-Supported Ruthenium Nanoparticles for Hydrogenation of Pyruvic Acid In the Aqueous Phase
AIChE Annual Meeting
2011
2011 Annual Meeting
Particle Technology Forum
Nanostructured Particles for Catalysis
Tuesday, October 18, 2011 - 10:15am to 10:36am
Heterogeneous catalysis is an important technology in the chemical industry. Incorporation of nanoscience into catalysis provides one of the most powerful approaches to understanding reaction mechanisms and designing new-generation catalysts more efficienctly1. In this work, we present a strategy for design of monodisperse Ruthenium nanoparticles (RuNPs), immobilization of the RuNPs onto ordered mesoporous silica (MSUF), and reactivity assessment of the supported catalyst (RuNPs/MSUF) by aqueous phase hydrogenation of pyruvic acid to lactic acid. The RuNPs were prepared by a polyol reduction method2 using ruthenium(III) acetylacetonate and poly(vinylpyrrolidone) (PVP) as precursor and stabilizer, respectively. Transmission electron microscopy (TEM) characterization showed that the particles were spherical with a fairly narrow size distribution and an average diameter of 3.5±0.5 nm. RuNPs/MSUF was prepared by immobilizing the RuNPs onto ordered mesoporous silica support MSUF using sonication method. RuNPs/MSUF was prepared by immobilizing the RuNPs onto ordered mesoporous silica support MSUF using sonication. TEM characterization showed well-dispersed particles on the surface of MSUF with no agglomeration and no damage to the framework of the support. Both inductively coupled plasma-atomic emission spectroscopy (ICP-AES) and X-ray photoelectron spectroscopy (XPS) characterization confirmed the attachment of RuNPs to MSUF. The reactivity of RuNPs/MSUF was evaluated by aqueous phase hydrogenation of pyruvic acid. All the reactions were conducted in a multi-batch reactor system (Parr Instrument Co., Model 5000), and the samples were analyzed by HPLC (Waters Co.) with an RI detector. A differential approach was used to compute the initial turnover frequency (TOF) for each reaction3,4. Results showed that, even under much milder reaction conditions than reported to-date5, the initial TOF of the reaction (685.2 h-1) catalyzed by RuNPs/MSUF is more than 25 times higher than values reported in the literature (24.2 h-1)5. It is also noteworthy that RuNPs/MSUF shows a significant improvement in TOF compared to commercial Ru catalysts, which is an indication of a higher utility efficiency of Ru in catalysis.
References:
- Gabor A. Somorjai, Feng Tao, et al. Top Catal (2008) 47:1–14
- Sang Hoon J, Jeong Y. Park, et al. Nano Lett., 2010, 10 (7), pp 2709–2713
- Zhang, Z.; Jackson, J. E.; Miller, D. J. Ind. Eng. Chem. Res., 2002, 41, 691-696.
- Mehmet Zahmakýran, et al. J. Am. Chem. Soc., 2010, 132 (18), pp 6541–6549
- R.. Luque, J.H. Clark. Catalysis Communications 11 (2010) 928–931