The electrosynthesis of ethylene oxide in a tandem recycle flow reactor system

被引:5
|
作者
Schalck, Jonathan [1 ,2 ]
Hereijgers, Jonas [1 ]
Guffens, Wim [2 ]
Breugelmans, Tom [1 ]
机构
[1] Univ Antwerp, Res Grp Appl Electrochem & Catalysis, Univ Pl 1, B-2610 Antwerp, Belgium
[2] BASF Antwerp NV, Scheldelaan 600, B-2040 Antwerp, Belgium
关键词
Ethylene oxide; Bromine mediated electrosynthesis; Recycling flow in tandem reactors; Electrochemical reactor engineering; CHLORINE EVOLUTION; OXIDATION; SELECTIVITY; MECHANISM; TITANIUM; CATALYST; OXYGEN;
D O I
10.1016/j.cej.2023.144741
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this work an electrochemical tandem recycle reactor was developed for the selective electro-oxidation of ethylene into ethylene oxide with a concentrated product outflow, resulting in an more sustainable pathway towards EO as opposed to the partial oxidation process. The system consisted of (i) a cation exchange membrane equipped module operating at a constant setpoint of 133.3 mA/cm2 and (ii) an anion exchange membrane unit in sequence, with a variable setpoint to regulate the pH. An excess of ethylene was supplied to the porous anode of the cation exchange module, which subsequently reacted with evolved bromine into 2-bromoethanol. As a result the anolyte acidified, which in turn promoted a selective bromine production. The anion exchange module also contributed to the Br2 production, converted 2-bromoethanol into ethylene oxide and neutralized the anolyte. The system underwent equal charge experiments in varied anolyte concentrations with a (i) Ni gauze cathode and an IrO2 coated Ti anode in the cation exchange module and (ii) graphite electrodes in the anion exchange unit. For experiments of 6 up to 10 h, Faradaic efficiencies towards ethylene oxide of 80.2 & PLUSMN; 6% and 46.7 & PLUSMN; 4.5% were sustained in 0.5 M and 3 M KBr anolyte respectively. The reduced selectivity in augmented KBr concentrations was predominantly caused by organochemical thermodynamics, which provoked an increased 1,2-dibromoethane production. The highest ethylene oxide production was achieved in a 0.5 M KBr condition, i.e. 10 g/L, which is ten times higher than the maximum reported figure in literature. In terms of stability, pretreated anodes, i.e. baked at 450 degrees C in air prior to testing, showed no degradation before and after testing on SEM-EDS analyses, whereas untreated structures were susceptible to corrosion.
引用
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页数:10
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