Tresatayawed Anchale, Glinrun Peangpit, Autthanit Chaowat, Jongsomjit Bunjerd
Center of Excellence on Catalysis and Catalytic Reaction Engineering, Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University.
Department of Petrochemicals and Environmental Management, Faculty of Engineering, Pathumwan Institute of Technology.
J Oleo Sci. 2020;69(5):503-515. doi: 10.5650/jos.ess19220.
In the present work, the palladium (Pd) modification and supporting effect of W/TiO catalysts on catalytic ethanol dehydration to ethylene and diethyl ether were investigated. The Pd modification with different sequence of Pd and W impregnation on the catalysts was prepared by the incipient wetness impregnation technique. The catalyst characterization and activity testing revealed that the different sequence during impregnation influenced the physicochemical properties and ethanol conversion of catalyst. The differences in structure and surface properties were investigated by XRD, BET, SEM, EDX, XPS and NH-TPD. Upon the reaction temperature between 200 to 400°C, it was found that the conversion increased with increasing of temperature for all catalysts. The Pd incorporated into catalysts enhanced the ethanol conversion depending on the sequence of impregnation. At low temperature (ca. 200 to 300°C), diethyl ether is a major product and the Pd modification over W/TiO catalyst resulted in increased diethyl ether yield. This is because an increase of ethanol conversion was obtained with Pd modification, while diethyl ether selectivity did not change. This can be attributed to the higher amount of weak acids sites present after Pd modification into catalyst. Among all catalysts, the PdW/TiO catalyst (coimpregnation) achieved the highest diethyl ether yield of 41.4% at 300℃. At high temperature (ca. 350 to 400°C), ethylene is the major product. The W/Pd/TiO catalyst (with sequential impregnation of Pd on TiO followed by W) exhibited the highest ethylene yield of 68.1% at 400°C. It can be concluded that the modification of Pd onto W/TiO upon different sequence of Pd and W impregnation can improve the diethyl ether and ethylene yield in catalytic ethanol dehydration.
在本工作中,研究了W/TiO催化剂上钯(Pd)的改性及其对乙醇催化脱水制乙烯和乙醚的负载效应。采用初湿浸渍法制备了钯和钨浸渍顺序不同的钯改性催化剂。催化剂表征和活性测试表明,浸渍过程中的不同顺序影响了催化剂的物理化学性质和乙醇转化率。通过XRD、BET、SEM、EDX、XPS和NH-TPD研究了结构和表面性质的差异。发现在200至400°C的反应温度下,所有催化剂的转化率均随温度升高而增加。引入催化剂中的钯根据浸渍顺序提高了乙醇转化率。在低温(约200至300°C)下,乙醚是主要产物,W/TiO催化剂上的钯改性导致乙醚产率增加。这是因为钯改性提高了乙醇转化率,而乙醚选择性没有变化。这可归因于钯改性后催化剂中存在的弱酸位点数量增加。在所有催化剂中,PdW/TiO催化剂(共浸渍)在300℃时实现了最高的乙醚产率,为41.4%。在高温(约350至400°C)下,乙烯是主要产物。W/Pd/TiO催化剂(先在TiO上浸渍Pd,然后浸渍W)在400°C时表现出最高的乙烯产率,为68.1%。可以得出结论,钯和钨浸渍顺序不同的情况下在W/TiO上进行钯改性可以提高乙醇催化脱水制乙醚和乙烯的产率。