Epoxidation of Butadiene Over Nickel Modified TS-1 Catalyst
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Epoxidation of Butadiene Over Nickel Modified TS-1 Catalyst Mei Wu • Lingjun Chou • Huanling Song
Received: 15 December 2011 / Accepted: 29 February 2012 / Published online: 21 March 2012 Ó Springer Science+Business Media, LLC 2012
Abstract Nickel modified Titanium silicalite 1 (TS-1) catalysts provided an environmentally benign and effective method for butadiene epoxidation. Certain loading of modified Ni in our system significantly promoted TS-1 catalytic activity. The product vinyloxirane (VO) was obtained with high yield of 0.49 mol/L (theoretic equilibrium value 0.52 mol/L). The turnover number (TON, determined as the molar VO obtained per molar Ti atom) reached 1,140. Besides, the catalyst kept high activity during five runs of reusability test. XRD, N2 adsorption and desorption, TPR, XPS, FT-IR and DR UV–Vis were employed to characterize the specific Ni role to Ti-site in Ni/TS-1 catalysts. Keywords Butadiene Epoxidation Vinyloxirane Titanium silicalite 1 Nickel
1 Introduction The epoxidation of butadiene (BD) is a typical atom economic reaction in respect of the activation of C=C bond [as shown in Eq. (1)]. The product vinyloxirane (VO) exhibits the characteristics of both alkenes and epoxides because of its two functional groups (carbon–carbon double bond and
M. Wu L. Chou H. Song (&) State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, People’s Republic of China e-mail: [email protected] M. Wu Graduate School of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
oxirane) in one molecule, and thus shows great value as an intermediate in synthesizing organic chemistry and chemical technology [1]. A variety of fine and special chemicals such as 2-amino-3-butene-1-ol, butylenes carbonate etc. can be obtained from VO. Conventionally, VO is prepared by the hydrolysis of BD monochlorohydrin (1-chloro-3butylene-2-ol) in alkaline media; BD monochlorohydrin is usually obtained through the oxidation of BD with hypochlorous acid [2]. This process has many disadvantages in regard of environmental and economic considerations.
ð1Þ In 1990s, Monnier prepared VO via the epoxidation of BD using oxygen or oxygen-containing gases as oxidant over silver catalysts (Ag/Al2O3), which made the synthesis of VO economical and environmental friendly [3]. Subsequently, a large number of investigations on Ag/Al2O3 system including catalysts and reaction mechanisms had been reported [1, 4–6]. In our previous work, the stability and activity of Ag/Al2O3 catalysts were greatly improved by IA/IIA metals [7]. However, the VO single-pass yield was relatively low, and deep oxidations of VO were inevitable at high temperature ([200 °C). Invention of titanium containing molecular sieves TS-1 by Taramasso et al. [8] opened a new route for catalytic reactions. For the unique pore-channel structure, TS-1 exhibits outstanding properties of shape selective catalysis oxidation. A lot of oxidation reactions with hydroge
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