Slurry loop tubular membrane reactor for the catalysed aerobic oxidation of benzyl alcohol

Slurry loop tubular membrane reactor for the catalysed aerobic oxidation of benzyl alcohol
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用于苯甲醇催化好氧氧化的浆液环路管式膜反应器

DOI:
10.1016/j.cej.2019.122250
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发表时间:
2019
影响因子:
15.1
通讯作者:
Venezia B
Venezia B
中科院分区:
工程技术1区
文献类型:
--
作者:
Venezia B

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设计了一种新颖的反应器,该反应器结合了在环路配置内流动的催化剂浆料,并结合了用于控制氧气输送的管式膜(Teflon AF-2400),并用于使用 1wt% Au-Pd/TiO2 粉末催化剂对苯甲醇进行有氧氧化。该反应器保持液相中氧气饱和,同时避免其中产生气泡,从而提高了操作安全性。与传统高压釜相比,间歇模式的实验结果表明,浆料环路膜反应器达到了相似的氧化周转频率(20,000–25,000h−1),苯甲醛选择性值相当(∼70%)。通过使用连接到环路的错流过滤器以防止催化剂离开反应器来实现连续操作。使用60cm长的管式膜,浆液流量以10mL/min循环,在100-120℃、0-5bar氧气压力和1.2-5.0g/L催化剂负载量下进行连续反应。通过降低反应温度或增加外部氧气压力来提高对苯甲醛的选择性。耗氧率随催化剂负载量线性下降,表明气液传质阻力可以忽略不计。通过将管状膜的长度加倍进一步证明了这一点,这对氧化周转频率没有影响。浆料环管膜反应器表现出明显优于填充床膜微通道反应器的性能,并且与滴流床毛细管反应器的性能相似。该反应器可用于广泛的应用,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。
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/TiO2powdered 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.
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