Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2019-07-15 , DOI: 10.1016/j.cej.2019.122250 Baldassarre Venezia , Mark Douthwaite , Gaowei Wu , Meenakshisundaram Sankar , Peter Ellis , Graham J. Hutchings , Asterios Gavriilidis
A novel reactor that combines a catalyst slurry flowing inside a loop configuration, incorporating a tubular membrane (Teflon AF-2400) for controlled oxygen delivery was designed and employed for the aerobic oxidation of benzyl alcohol using a 1 wt% Au-Pd/TiO2 powdered catalyst. This reactor keeps the liquid phase saturated with oxygen, while avoiding the creation of bubbles in it, thus enhancing operation safety. Experimental results in batch mode compared with those of a conventional autoclave demonstrated that the slurry loop membrane reactor reached a similar oxidation turnover frequency (20,000–25,000 h−1) with comparable values of benzaldehyde selectivity (∼70%). Continuous operation was achieved by using a crossflow filter connected to the loop to keep the catalyst from exiting the reactor. Using a 60 cm long tubular membrane, with the slurry flow circulating at 10 mL/min, continuous reaction was performed at 100–120 °C, 0–5 bar oxygen pressure and 1.2–5.0 g/L catalyst loading. Selectivity to benzaldehyde increased by either decreasing the reaction temperature or increasing the external oxygen pressure. The oxygen consumption rate decreased linearly with the catalyst loading, suggesting negligible gas-liquid mass transfer resistance. This was further evidenced by doubling the length of the tubular membrane, which had no effect on the oxidation turnover frequency. The slurry loop membrane reactor showed significantly better performance than packed-bed membrane microchannel reactors, and similar performance as that of a trickle-bed capillary reactor. This reactor can be implemented for a wide range of applications, which rely on the use of powder catalyst, are limited by gaseous reactant availability and require safe operation.
中文翻译:
用于苯甲醇的好氧氧化的浆料回路管式膜反应器
设计了一种新颖的反应器,该反应器结合了在环形结构内流动的催化剂浆料,并结合了用于控制氧气输送的管状膜(Teflon AF-2400),并用于使用1 wt%的Au-Pd / TiO 2进行苄醇的好氧氧化粉末状催化剂。该反应器使液相保持氧饱和,同时避免在其中产生气泡,从而提高了操作安全性。与常规高压釜相比,分批模式的实验结果表明,淤浆环膜反应器达到了相似的氧化转换频率(20,000–25,000 h -1)具有可比的苯甲醛选择性值(约70%)。通过使用连接到回路的错流过滤器以保持催化剂不离开反应器来实现连续操作。使用60厘米长的管状膜,使浆液以10 mL / min的速度循环,在100–120°C,0–5 bar的氧气压力和1.2–5.0 g / L的催化剂负载下进行连续反应。通过降低反应温度或增加外部氧气压力,可以提高对苯甲醛的选择性。氧消耗速率随催化剂负载量线性降低,表明气液传质阻力可忽略不计。通过使管状膜的长度加倍而进一步证明了这一点,这对氧化转换频率没有影响。淤浆环流膜反应器显示出比填充床膜微通道反应器明显更好的性能,并且与滴流床毛细管反应器具有相似的性能。该反应器可实现广泛的应用,这些应用依赖于粉末催化剂的使用,受到气态反应物可用性的限制,并且需要安全操作。