Ni/NaX: A Bifunctional Efficient Catalyst for Selective Hydrogenolysis of Glycerol
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Ni/NaX: A Bifunctional Efficient Catalyst for Selective Hydrogenolysis of Glycerol Jing Zhao • Weiqiang Yu • Chen Chen Hong Miao • Hong Ma • Jie Xu
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Received: 22 May 2009 / Accepted: 30 October 2009 / Published online: 14 November 2009 Ó Springer Science+Business Media, LLC 2009
Abstract Non-noble metal Ni/NaX catalyst was prepared and used in the hydrogenolysis of aqueous glycerol. Characterization by XRD, SAED, H2 chemisorption, ICP and NH3-TPD techniques disclosed that the proper strong acid sites were responsible for the high activity and selectivity. Over Ni/NaX catalyst, conversion of glycerol reached 86.6% with 94.6% selectivity to glycols including 1,2-proplyene glycol and ethylene glycol under 6.0 MPa H2 pressure at 200 °C after 10 h reaction. Additionally, the effects of time, temperature, and H2 pressure were investigated in detail. Keywords Glycerol Hydrogenolysis Nickel NaX zeolite Acidity
1 Introduction Due to the decrease of fossil resources and the increase of atmospheric carbon dioxide caused by fuel combustion, catalytic conversion of renewable biomass-derived materials into value-added oxygenated chemicals has attracted more and more attention. Glycerol, one of the top-12 Electronic supplementary material The online version of this article (doi:10.1007/s10562-009-0208-4) contains supplementary material, which is available to authorized users. J. Zhao W. Yu C. Chen H. Miao H. Ma J. Xu (&) State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, 116023 Dalian, People’s Republic of China e-mail: [email protected] J. Zhao W. Yu Graduate University of Chinese Academy of Sciences, 100049 Beijing, People’s Republic of China
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building block chemicals [1], is a main byproduct (10 wt%) in biodiesel production by transesterification of vegetable oils [2], which is available in large quantities accompanying the increase of biodiesel production. To enhance the economy of the whole biodiesel industry, various processes have been developed to catalytically convert glycerol to value-added chemicals [3, 4]. Among these processes, hydrogenolysis of glycerol to 1,2-propylene glycol (1,2-PG) and ethylene glycol (EG) is very fascinating. Both glycols are important chemical feedstocks, which are mostly used in the production of intermediates such as unsaturated resin and epoxy resin [5, 6]. At present, they are mainly produced from non-renewable petroleum derivatives such as propylene or ethylene. Compared with this traditional method, the process of obtaining these two glycols from renewable glycerol is more sustainable and green, and will be rapidly developed under the present situation. In literature, various catalysts, mainly based on noble metals such as Ru, Rh, and Pt [5–9], were reported for the hydrogenolysis of glycerol. Miyazawa et al. [7] found a metal–acid catalyst system, combining 5% Ru/C and Amberlyst-15, which was active in the hydrogenolysis reaction with 55% selectivity of 1,2-PG and 13% conversion. Alhanash e
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