Gas phase glycerol conversion over lanthanum based catalysts: LaNiO3 and La2O3

Gas phase glycerol conversion over lanthanum based catalysts: LaNiO3 and La2O3
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DOI:
10.1016/j.apcata.2013.07.016
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发表时间:
2013-10-02
影响因子:
5.5
通讯作者:
Batiot-Dupeyrat, Catherine
Batiot-Dupeyrat, Catherine
中科院分区:
化学2区
文献类型:
--
作者:
Hernandez, Diana;Velasquez, Mauricio;Batiot-Dupeyrat, Catherine

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考察了La系催化剂LaNiO_3和La_2O_3在甘油气相转化反应中的催化性能。该反应在300-700℃范围内进行,在400℃和500℃时,有利于在液体中生成化合物,而在高温下,主要生成一氧化碳、二氧化碳和氢气等气体。本研究使用的碱性催化剂有利于羟基丙酮的生产。此外,还生成了大量的1,2丙二醇、甲醇和乙二醇。钙钛矿型LaNiO_3和La_2O_3在400℃下10h内没有明显的失活现象,羟丙酮的选择性随着反应时间的延长而略有下降,很可能是由于重质产物的形成。对反应前后的催化剂进行了表征(X射线衍射、热重分析、CO2-TPD),结果表明,在400℃的反应中,LaNiO_3被部分还原为LaNiO_2·5。与LaNiO_3相比,La_2O_3的强碱性中心对甘油醛、乙醛、丙醛和丙酮合成甲醇的催化活性特别高。(C)2013年提交人。爱思唯尔出版,版权所有。
The catalytic performance of lanthanum based catalysts: LaNiO3 and La2O3 were evaluated in the gas-phase transformation of glycerol. The reaction was investigated in the temperature range of 300-700 degrees C. At 400 and 500 degrees C, the production of compounds in liquid phase is favored while at high temperature gases such as carbon monoxide, carbon dioxide and hydrogen are mainly formed. The basic catalysts used in this study favor the production of hydroxyacetone. Additionally 1,2 propanediol, methanol and ethylene glycol were formed in significant amount. The perovskite LaNiO3 and La2O3 show no significant deactivation during 10 h at 400 degrees C, the selectivity to hydroxyacetone only slightly decreased with time on stream most probably due to the formation of heavy products. The catalysts were characterized before and after reaction (XRD, TGA, CO2-TPD) showing that LaNiO3 was partially reduced into LaNiO2.5 during reaction at 400 degrees C. It is suggested that strong basic sites of La2O3 compared to LaNiO3 are particularly active to produce methanol through glyceraldehyde but also acetaldehyde, propionaldehyde and acetone. (C) 2013 The Authors. Published by Elsevier B.V. All rights reserved.