Sulfur removal from ionic liquid-assisted coal water slurry electrolysis in KNO3 system
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摘要: 在稳流条件下,考察了KNO3体系中离子液体辅助煤浆电解脱硫效果.研究了煤浆电解过程中离子液体结构、浓度、温度和时间对脱硫率的影响.当咪唑类离子液体有机结构相同时,不同阴离子脱硫率由高到低顺序为:Br- >BF4- >Cl-;当阴离子同为Br-时,咪唑脱硫效果优于吡啶.随着吡啶类离子液体([BPy]Br)浓度增加,脱硫率先增加,在0.3 mol/L处达到最大值,而后下降.此外,脱硫率随温度和时间增加而增大.最后,通过X射线光电子能谱(XPS)分析技术对实验前后煤中有机硫形态进行了分析.结果表明,噻吩主要通过萃取-氧化反应脱除,而其他形式有机硫(如硫醚、亚砜)则主要通过促进氧化及水解反应脱除.Abstract: Ionic liquid-assisted coal water slurry (CWS) electrolysis was carried out in KNO3 system with constant current. The effects of ionic liquids including structure, concentration, temperature and time on the removal of sulfur were investigated to intensify desulfurization ratio from CWS electrolysis. Given the organic structure of imidazole, the influence of anions on the desulfurization was in the following order: Br->BF4- >Cl-. Given the same anion of Br-, imidazole showed better performance than pyridine in terms of sulfur elimination. With increasing N-butylpyridinium bromide ([BPy]Br) concentration, the desulfurization ratio increased at the initial stage, and then decreased after 0.30 mol/L. Additionally, the desulfurization ratio continuously increased with time and temperature. Finally, the organic sulfur occurrences in coal before and after experiments were characterized by XPS technique. Results showed that the removal of thiophene was improved due to the extraction-oxidation effects and others (i.e. thioethers and sulfoxide) were removed mainly via enhanced oxidation and hydrolysis reactions.
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Key words:
- coal water slurry /
- electrolysis /
- ionic liquids /
- sulfur
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