A high pressure single-pass high-conversion electrochemical cell for intensification of organic electrosynthesis processes
A high pressure single-pass high-conversion electrochemical cell for intensification of organic electrosynthesis processes
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DOI：
10.1016/j.ces.2010.11.002
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发表时间：
2011-02-01
影响因子：
4.7
通讯作者：
Lapicque, Francois
中科院分区：
文献类型：
--
作者：
Attour, Anis;Dirrenberger, Patricia;Lapicque, Francois
以4-甲氧基甲苯（4-MT）在甲醇中阳极氧化制备4-甲氧基苄基二甲基缩醛（4-MBDMA）为实验反应，研究了在单程高转化率模式下连续运行的微通道电化学反应器。该电池由两个不锈钢阴极组成，在平坦的玻璃碳阳极周围开槽有100 mm深的通道。在电解槽中施加高达20巴的压力，以降低阴极产生的氢气的体积流速。狭窄的间隙和在压力下的操作导致电池的电解质电导率的增强，并且使得可以使用浓溶液、高电流密度和非常低的支持电解质浓度（即0.01 M KF）来操作电池性能从电池电压、反应物转化率、材料和电流效率以及最终在4-MBDMA中的选择性方面进行讨论。研究了进口试剂浓度、压力、流量和温度对反应的影响。在5巴和45 ℃下使用0.5 M 4-MT获得最佳性能：对于90%的转化率，选择性和电流效率分别达到92%和85%。在这种情况下，高压、单程高转化率电池表现出比当前工业方法高5-10倍的时空产率，并且支持电解质的浓度显著更低。(C)2010爱思唯尔有限公司版权所有。
The anode oxidation of 4-methoxytoluene (4-MT) to 4-methoxybenzyl dimethylacetal (4-MBDMA) in methanol is used as a test reaction for the study of a microchannel electrochemical reactor operated continuously in a single-pass high-conversion mode. The cell consists of two stainless steel cathodes, grooved with 100 mm deep channels surrounding a flat glassy carbon anode. Pressures up to 20 bars are applied in the cell in order to reduce the volumetric flow rate of the cathodically produced hydrogen. Both the narrow gap and the operation under pressure lead to an enhancement of the electrolytic conductivity of the cell and make it possible to operate with concentrated solutions, with high current densities and with a very low supporting electrolyte concentration (i.e. 0.01 M KF).The cell performance is discussed in terms of cell voltage, reactant conversion, material and current efficiency and finally selectivity in 4-MBDMA. The effect of inlet reagent concentration, pressure, flow-rate and temperature are investigated. Best performance is obtained with 0.5 M 4-MT at 5 bars and 45 degrees C: for a 90% conversion, selectivity and current efficiency attain, respectively, 92% and 85%. The high pressure, single-pass high-conversion cell exhibits in this case a space time yield 5-10 times higher than the current industrial process, with a significantly lower concentration of the supporting electrolyte. (C) 2010 Elsevier Ltd. All rights reserved.