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Butadiene from ethanol employing doped t-ZrO2
Molecular Catalysis ( IF 3.9 ) Pub Date : 2018-02-01 , DOI: 10.1016/j.mcat.2018.01.018
Luciano H. Chagas , Caio R.V. Matheus , Priscila C. Zonetti , Lucia G. Appel

The synthesis of 1,3-butadiene (BD) from ethanol is a complex reaction system in which several steps are involved. The use of zirconia-based catalysts as well as physical mixtures containing Cu/ZnO/Al2O3 (CZA) and t-ZrO2 were evaluated in order to better understand this reaction. The catalysts employed were characterized by the following techniques: TPSR-IR, NH3-TPD, CO2-TPD, XRD, SEM/EDS and BET. Moreover, the isopropanol conversion and the acetone and ethanol reaction (Meerwein-Ponndorf-Verley mechanism (MPV)) were used as model reactions to describe the catalysts behavior. It was verified that doping oxides with metals is a very simple procedure in order to change the properties of the catalysts so as to reach the requirements of the butadiene synthesis. Doped t-ZrO2-based catalysts are promising systems for the BD generation from ethanol. The addition of Na and Ag to t-ZrO2 promotes the selectivity towards BD and decreases the selectivity to ethylene. The catalyst with Ag is more active than the one with Na. It was observed that employing physical mixtures, the dehydrogenation rate of ethanol should be consistent with the activity of the catalyst toward the aldol condensation and the MPV step. The physical mixture with low concentration of CZA generates high BD yield. The ZrO2 catalytic behavior in the MPV step, and also in the BD synthesis changes according to the crystalline structure of this oxide.



中文翻译:

来自乙醇的丁二烯,采用掺杂的t -ZrO 2

由乙醇合成1,3-丁二烯(BD)是一个复杂的反应系统,其中涉及多个步骤。为了更好地理解该反应,对氧化锆基催化剂以及含有Cu / ZnO / Al 2 O 3(CZA)和t -ZrO 2的物理混合物的使用进行了评估。所采用的催化剂通过以下技术进行表征:TPSR-IR,NH 3 -TPD,CO 2 -TPD XRD,SEM / EDS和BET。此外,以异丙醇转化和丙酮和乙醇反应(Meerwein-Ponndorf-Verley机制(MPV))作为模型反应来描述催化剂的行为。已经证实,用金属掺杂氧化物是非常简单的程序,以改变催化剂的性能,从而达到丁二烯合成的要求。掺杂的基于t- ZrO 2的催化剂是从乙醇生成BD的有前途的系统。向t- ZrO 2中添加Na和Ag促进了对BD的选择性并降低了对乙烯的选择性。具有Ag的催化剂比具有Na的催化剂更具活性。观察到,采用物理混合物,乙醇的脱氢速率应与催化剂对醛醇缩合和MPV步骤的活性相一致。CZA浓度低的物理混合物可产生高BD产量。MPV步骤以及BD合成中的ZrO 2催化行为根据该氧化物的晶体结构而变化。

更新日期:2018-02-01
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