高等学校化学学报 ›› 2014, Vol. 35 ›› Issue (4): 760.doi: 10.7503/cjcu20130734

• 有机化学 • 上一篇    下一篇

有机胺型铁基离子液体的H2S吸收和再生性能

马云倩, 王睿()   

  1. 山东大学环境科学与工程学院, 济南 250100
  • 收稿日期:2013-07-31 出版日期:2014-04-10 发布日期:2013-09-17
  • 作者简介:联系人简介: 王 睿, 男, 博士, 教授, 博士生导师, 主要从事环境污染物治理研究. E-mail: ree_wong@hotmail.com
  • 基金资助:
    国家自然科学基金(批准号: 21276144)、 教育部科技重点项目(批准号: 109094)和博士点基金优先发展领域课题(批准号: 20110131130001)资助

H2S Absorption Capacity and Regeneration Performance of Amine Fe-based Ionic Liquid

MA Yunqian, WANG Rui*()   

  1. School of Environmental Science and Engineering, Shandong University, Jinan 250100, China
  • Received:2013-07-31 Online:2014-04-10 Published:2013-09-17
  • Contact: WANG Rui E-mail:ree_wong@hotmail.com
  • Supported by:
    † Supported by the National Natural Science Foundation of China(No.21276144), the Scientific Key Project from Chinese Ministry of Education(No.109094), and the Ph.D.Program Project for Priority Development Field from Chinese Ministry of Education(No.20110131130001)

摘要:

合成了有机胺型铁基离子液体1.6Et3NHCl·FeCl3, 研究了其热稳定性和对H2S的吸收与再生性能. 考察了H2S浓度为832 mg/m3, 温度为40~180 ℃, 气体流速分别为100, 300, 400和500 mL/min条件下H2S的去除率, 结果表明当气体流速小于400 mL/min时, 吸收率可达100%; 随着温度升高, 吸收效率提高并趋于恒定. 在最优条件下测得1.6Et3NHCl·FeCl3离子液体的硫容量为6.36 g/L, 远高于[Bmim]FeCl4离子液体. 通过比较吸收H2S前后的红外光谱图, 进一步确定了氧化反应的发生. 采用密度泛函理论从分子水平上研究了H2S与1.6Et3NHCl·FeCl3和[Bmim]FeCl4两种铁基离子液体以及Fe3+水溶液的相互作用, 从理论上比较了脱硫剂中的基质对H2S吸收的影响, 确定了胺基对H2S吸收的促进作用. 通过对脱硫产物的XRD分析, 确定了斜方晶体(α-硫)的生成, 与传统水相湿法氧化脱硫得到的产物相同. 通入空气可快速有效地对1.6Et3NHCl·FeCl3离子液体进行再生.

关键词: 硫化氢, 有机胺型铁基离子液体, 湿法氧化

Abstract:

Amine Fe-based ionic liquid 1.6Et3NHCl·FeCl3 was synthesized with ideal H2S absorption capacity and good thermostability. H2S removal efficiency was tested under the condition with H2S concentration of 832 mg/m3, temperature ranging from 40 ℃ to 180 ℃, and gas flow of 100, 300, 400 or 500 mL/min. The results showed that when the gas flow was less than 400 mL/min, H2S removal efficiency could reach 100%; H2S removal efficiency increased with the increasing in temperature and tended to approach an asymptotic value. Under the optimal conditions, the sulfur capacity of 1.6Et3NHCl·FeCl3 was 6.36 g/L, higher than that of [Bmim]FeCl4. Comparing the FTIR spectra before and after H2S absorption, redox reaction between 1.6Et3NHCl·FeCl3 and H2S was confirmed. The interaction between H2S and 1.6Et3NHCl·FeCl3/[Bmim]FeCl4/H2O has been studied at the molecular level using density functional theory, and the influence of the substrate on H2S absorption was illustrated to be responsible for the enhancement of H2S absorption by aminal group. The product after H2S absorption was orthorhombic crystal sulfur(α), which is the same as the product from traditional aqueous phase oxidation desulfurization. 1.6Et3NHCl·FeCl3 ionic liquid can be reused efficiently after quick regeneration by air flow.

Key words: H2S, Amine Fe-based ionic liquid, Wet oxidation

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