1,3-Butadiene Production by Crotyl Alcohol Dehydration over Solid Acids and Catalyst Deactivation by Water Adsorption
1,3-Butadiene Production by Crotyl Alcohol Dehydration over Solid Acids and Catalyst Deactivation by Water Adsorption
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固体酸巴豆醇脱水生产 1,3-丁二烯及水吸附催化剂失活
DOI：
10.1627/jpi.63.70
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发表时间：
2020
影响因子：
1
通讯作者：
M. Okamoto
中科院分区：
文献类型：
--
作者：
A. Segawa;Tatsuya Ichijo;Nobuhiro Kimura;Keisuke Tsuruta;N. Yoshida;M. Okamoto
研究了固体酸催化巴豆醇（2-丁烯-1-醇）脱水合成1，3-丁二烯。在工业硅铝催化剂上，丁烯醇转化率和丁二烯选择性均在95%以上.然而，在反应过程中观察到催化活性的突然降低。根据失活催化剂在150-200 ℃下干燥再生的事实，揭示了催化剂失活的主要原因是反应过程中形成的水的吸附，而不是焦炭的形成。对失活催化剂的分析表明，由于Al _ O _ Al键水解生成的Al _ OH增加了催化剂表面的亲水性，从而促进了水在催化剂表面的吸附，而抑制了巴豆醇在催化剂表面的吸附。此外，在催化剂表征的基础上，得出的结论是，硅醇基团少，富铝区少，低硅铝比的硅铝催化剂是优选的。
We studied the synthesis of 1,3-butadiene via the dehydration of crotyl alcohol (2-buten-1-ol) over solid acids. Crotyl alcohol conversion and butadiene selectivity were both 95 % or more over commercial silica _ alumina catalysts. However, a sudden decrease in catalytic activity was observed during the reaction. On the basis of the fact that the deactivated catalyst was regenerated by drying at 150-200 °C, it was revealed that the main cause of the catalyst deactivation was the adsorption of water formed during the reaction and not the coke formation. An analysis of the deactivated catalyst indicated that, since the formation of Al _ OH by the hydrolysis of the Al _ O _ Al bond increased the hydrophilicity of the catalyst surface, the adsorption of water on the catalyst surface was pro-moted, whereas that of crotyl alcohol was probably inhibited. Moreover, on the basis of the catalyst characterization, it was concluded that silica _ alumina catalysts with few silanol groups, few alumina-rich zones, and a low Si/Al ratio were preferable.