Formation of 1,3-butadiene from ethanol in a two-step process using modified zeolite-β catalysts
Formation of 1,3-butadiene from ethanol in a two-step process using modified zeolite-β catalysts
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DOI：
10.1016/j.apcata.2016.01.026
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发表时间：
2016-03-25
影响因子：
5.5
通讯作者：
Palkovits, Regina
中科院分区：
文献类型：
--
作者：
Klein, Alexander;Keisers, Kristina;Palkovits, Regina
在连续两段气相固定床反应器装置中，开发了用于乙醇选择性生成1，3-丁二烯的催化剂。在第一阶段中，期望20%的乙醛产率。将该混合物直接进料到第二阶段中，以促进对1，3-丁二烯的选择性的提高。在第一阶段，研究了Ag\SiO2和Cu\SiO2。特别是铜基催化剂被证明是一种选择性和长期稳定的体系。在第二阶段中，我们测试了不同的沸石-β基催化剂体系，所述催化剂体系在其酸性和碱性行为方面进行了改性。我们能够在573 K的相当低的温度下达到高达72%的1，3-丁二烯选择性。此外，我们可以得出催化剂的酸性和碱性性质与其催化性能之间的直接相关性。通过X射线衍射、氮气物理吸附、热重-差示扫描量热法和高分辨透射电镜分析了其物理性能。化学组成由ICP-AES和SEM-EDX测量确定。采用吡啶吸附红外光谱法和氨、二氧化碳程序升温脱附法分别研究了其酸碱性质。(C)© 2016 Elsevier B. V.版权所有。
Catalysts for the selective formation of 1,3-butadiene out of ethanol in a continuous two-stage gas-phase fixed bed reactor setup were developed. In the first stage, 20% acetaldehyde yield was aspired. This mixture was directly fed into the second stage facilitating enhanced selectivity to 1,3-butadiene. In the first stage, Ag\SiO2 and Cu \SiO2 were studied. Especially the copper based catalyst proved to be a selective and long-term stable system. In the second stage we tested different zeolite-beta based catalyst systems which were modified in terms of their acidic and basic behaviour. We were able to reach 1,3-butadiene selectivities up to 72% at rather low temperatures of 573 K. Furthermore we could draw a direct correlation between the catalyst's acidic and basic properties and their catalytic performance. The physical properties were analysed via X-ray diffraction, nitrogen physisorption, TGA-DSC and HRTEM. The chemical composition was determined by ICP-AES and SEM-EDX measurements. The investigation of the acidic and basic properties was realized by pyridine adsorption infrared spectroscopy and temperature programmed desorption with ammonia and carbon dioxide, respectively. (C) 2016 Elsevier B.V. All rights reserved.