Sustainable production of acrolein:: gas-phase dehydration of glycerol over 12-tungstophosphoric acid supported on ZrO2 and SiO2
Sustainable production of acrolein:: gas-phase dehydration of glycerol over 12-tungstophosphoric acid supported on ZrO2 and SiO2
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DOI：
10.1039/b805373a
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发表时间：
2008-01-01
期刊：
影响因子：
9.8
通讯作者：
Xu, Bo-Qing
中科院分区：
文献类型：
--
作者：
Chai, Song-Hai;Wang, Hao-Peng;Xu, Bo-Qing
研究了不同处理温度的负载型12-钨磷酸(H3PW12O40，HPW)催化剂在315℃下催化甘油气相脱水制丙烯醛的反应。用X射线衍射仪和拉曼光谱对所制备的HPW/SiO_2、HPW/ZrO_2催化剂进行了表征，结果表明，载体材料的性质对HPW的热稳定性有显著影响，经650℃热处理后，HPW在ZrO_2表面保持完整的Keggin结构，在SiO_2表面完全破坏。HPW在氧化锆上的分散度也高于在二氧化硅上的分散度。与HPW/SiO_2催化剂相比，HPW/ZrO_2催化剂具有更高的丙烯醛生成活性和选择性，并且在脱水反应中失活速度较慢。在较好的HPW/ZrO2催化剂上，即使在反应10h后，丙烯醛的选择性和产率也可以分别高达70mol%和54%。
Catalytic gas-phase dehydration of glycerol to produce acrolein was investigated at 315 degrees C over ZrO2-and SiO2-supported 12-tungstophosphoric acid (H3PW12O40, HPW) catalysts with different treatment temperatures. Characterizations with XRD and Raman spectroscopy of the prepared HPW/SiO2, HPW/ZrO2 catalysts showed that the nature of support materials had a significant effect on the thermal stability of HPW; after thermal treatment at 650 degrees C, the Keggin structure of HPW remained intact on the surface of ZrO2 but was completely destroyed on SiO2. HPW on ZrO2 also showed higher dispersion than on SiO2. In comparison to HPW/SiO2, HPW/ZrO2 catalysts exhibited significantly higher activity and selectivity for the formation of acrolein, as well as a slower deactivation rate during the dehydration reaction. The selectivity and yield for acrolein over the better HPW/ZrO2 catalysts can be as high as 70 mol% and 54%, respectively, even after 10 h reaction.