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Coating of Pd/C catalysts with Lewis-acidic ionic liquids and liquid coordination complexes–SCILL induced activity enhancement in arene hydrogenation

机译:刘易斯酸性离子液体和液体配位化合物对Pd / C催化剂的包覆作用– SCILL促进了芳烃加氢的活性

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摘要

New solid catalysts with ionic liquid layer (SCILLs) were prepared by the coating of heterogeneous Pd/C catalysts with a thin film of acidic liquid: a known chloroaluminate ionic liquid (IL), [BMIM]Cl/AlCl3, and a recently developed liquid coordination complex (LCC), urea/AlCl3. Both coatings improved the activity of Pd/C catalyst against toluene hydrogenation; at lower temperatures (40 °C) the IL-SCILL performed better, whereas at 80 °C the LCC-SCILL gave higher conversion. A thin film of ionic liquid proved to be sufficient to increase activity, while larger volumes of ionic liquid resulted in a decrease in activity due to pore blocking and hence mass transport limitations. Kinetic investigations in batch mode revealed a zero order with respect to toluene concentration, a first order in hydrogen pressure, and activation energy of 64.7 kJ mol−1 for the Pd/C catalyst. The SCILL catalysts had slightly lower values of 53.1 kJ mol−1 for [BMIM]Cl/AlCl3 and 61.4 kJ mol−1 for urea/AlCl3, respectively.
机译:通过用酸性液体薄膜涂覆异质Pd / C催化剂,可以制备出具有离子液体层(SCILLs)的新型固体催化剂:已知的氯铝酸盐离子液体(IL),[BMIM] Cl / AlCl3和最近开发的液体配位化合物(LCC),尿素/ AlCl3。两种涂层均提高了Pd / C催化剂对甲苯加氢的活性;在较低温度(40°C)下,IL-SCILL的性能更好,而在80°C下,LCC-SCILL的转化率更高。离子液体薄膜证明足以增加活性,而较大体积的离子液体则由于孔阻塞而导致活性降低,因此限制了质量传输。间歇模式下的动力学研究表明,对于Pd / C催化剂,甲苯浓度为零级,氢气压力为一级,活化能为64.7 kJ mol-1。对于[BMIM] Cl / AlCl3,SCILL催化剂的值略低一些,分别为53.1 kJ mol-1和对于尿素/ AlCl3的值分别为61.4 kJ mol-1。

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