Clean synthesis of alkyl levulinates from levulinic acid over one pot synthesized WO3-SBA-16 catalyst

Siva Sankar Enumula, Venkata Ramesh Babu Gurram, Raji Reddy Chada, David Raju Burri, Seetha Rama Rao Kamaraju
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引用次数: 65

Abstract

The present work highlights the application of solid acid catalyst to produce alkyl levulinate from levulinic acid in continuous mode under vapor phase conditions. In this context, tungsten oxide incorporated SBA-16 catalysts were prepared by one pot direct synthesis method and evaluated for the titled reaction. Under optimized reaction conditions, 3 wt% WO3-SBA-16 catalyst delivered complete conversion of levulinic acid with 95% selectivity towards ethyl levulinate. The synthesized catalysts were characterized to know the physico-chemical features by various techniques, namely, X-ray diffraction, N2 physisorption, temperature programmed reduction of hydrogen (H2-TPR), temperature programmed desorption of ammonia (NH3-TPD), DR-UV–vis spectroscopy, Fourier transform infrared (FTIR) spectroscopy, transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The characterization results suggest that, the superior catalytic activity can be ascribed due to the enhanced acidity of SBA-16 obtained through incorporation of tungsten oxide and easy of accessibility for the dispersed active sites through uniform pore channels. The constant catalytic activity in 10 h time on study shows the sturdiness of the catalyst and the spent catalyst can be regenerated several times. Moreover, various alkyl levulinates (methyl, n-propyl, and n-butyl) were synthesized with more than 90% selectivity over this catalyst.

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用一锅合成WO3-SBA-16催化剂催化乙酰丙酸清洁合成乙酰丙酸烷基酯
本工作重点介绍了固体酸催化剂在气相条件下由乙酰丙酸连续生产乙酰丙酸烷基的应用。在此背景下,采用一锅直接合成法制备了SBA-16氧化钨催化剂,并对反应进行了评价。在优化的反应条件下,3wt %的WO3-SBA-16催化剂实现了乙酰丙酸完全转化,乙酰丙酸乙酯的选择性为95%。采用x射线衍射、N2物理吸附、程序升温还原氢(H2-TPR)、程序升温解吸氨(NH3-TPD)、DR-UV-vis光谱、傅里叶变换红外(FTIR)光谱、透射电子显微镜(TEM)和扫描电子显微镜(SEM)等技术对合成的催化剂进行表征,了解催化剂的理化性质。表征结果表明,SBA-16之所以具有优异的催化活性,主要是由于加入氧化钨后SBA-16的酸性增强,分散的活性位点易于通过均匀的孔道接近。研究表明,该催化剂在10 h内具有稳定的催化活性,且废催化剂可多次再生。此外,在该催化剂上合成了各种乙酰丙酸烷基酯(甲基、正丙基和正丁基),选择性超过90%。
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期刊介绍: The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.
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