石油化工高等学校学报

石油化工高等学校学报

• 石油化工 • 上一篇    下一篇

溶剂pH对Ce⁃SBA⁃15吸附剂酸活性位构筑及脱硫性能的影响

郭忠森,龚珣,吕曼丽,张健,秦玉才,宋丽娟   

  1. (辽宁石油化工大学 辽宁省石油化工催化科学与技术重点实验室,辽宁 抚顺 113001)
  • 收稿日期:2019-04-17 修回日期:2019-05-14 出版日期:2019-10-31 发布日期:2019-10-30
  • 通讯作者: 宋丽娟(1962⁃),女,博士,教授,博士生导师,从事分子筛酸性及活性位催化性能与表征研究;E⁃mail:lsong56@263.net
  • 作者简介:郭忠森(1992-),男,硕士研究生,从事清洁燃料生产研究; E-mail:Guozhongsen1992@126.com
  • 基金资助:
    国家自然科学基金项目(U1662135)

The Effect of Solvent pH Value on Acid Active Site Construction and Desulfurization Performance of Ce⁃SBA⁃15 Desulfurization Adsorbent

The Effect of Solvent pH Value on Acid Active Site Construction and Desulfurization Performance of Ce?SBA?15 Desulfurization Adsorbent   

  1. (Key Laboratory of Petrochemical Catalytic Science of Liaoning Province, Liaoning Shihua University,Fushun Liaoning 113001,China)
  • Received:2019-04-17 Revised:2019-05-14 Online:2019-10-31 Published:2019-10-30
  • Supported by:
    (Key Laboratory of Petrochemical Catalytic Science of Liaoning Province, Liaoning Shihua University,Fushun Liaoning 113001,China)

摘要: 采用浸渍法制备Ce⁃SBA⁃15吸附剂,运用N2吸附⁃脱附技术和NH3⁃TPD技术表征吸附剂的物化性质,采用静态吸附实验、固定床动态吸附穿透实验和萃取实验考察吸附剂的脱硫效果。将吸附剂物化性质和脱硫效果相关联,考察制备过程中溶剂pH对Ce⁃SBA⁃15吸附剂酸活性位构筑及脱硫性能的影响。研究表明,溶剂的pH对Ce⁃SBA⁃15脱硫吸附剂酸活性位的构筑存在强静电吸附作用和氧化还原作用两种影响。强酸性条件能够抑制氧化反应的发生,同时由于强静电吸附作用实现Ce物种的高度分散。弱酸性条件由于氧化反应的发生导致Ce物种发生转化而难以形成有效噻吩吸附活性位。最佳的pH为3,此条件下制备的Ce⁃SBA⁃15(3)吸附剂保持有最优的物化性质和噻吩吸附脱除能力。

关键词: Ce?SBA?15, pH, 活性位, 吸附脱硫

Abstract: The Ce⁃SBA⁃15 adsorbent was prepared by impregnation method. The physicochemical properties of the adsorbent were characterized by N2 adsorption⁃desorption technique and NH3⁃TPD technique. The desulfurization effect of adsorbent was investigated by static adsorption experiment, fixed bed dynamic adsorption penetration experiment and extraction experiment. The physical and chemical properties of the adsorbent were correlated with the desulfurization effect, and the influence of the solvent pH value on the acid active site construction and desulfurization performance of Ce⁃SBA⁃15 adsorbent was investigated. The results showed that the pH value of the solvent had two effects (the strong electrostatic adsorption and oxidation reaction ) on the construction of acid active sites of Ce⁃SBA⁃15 desulfurization adsorbent. Strong acidic conditions can inhibit the occurrence of oxidation reaction, and high dispersion of Ce species can be achieved due to strong electrostatic adsorption. Under weak acidic conditions, it is difficult to form effective thiophene adsorption sites due to the transformation of Ce species caused by oxidation. The optimal pH value was 3, and the Ce⁃SBA⁃15(3) adsorbent prepared under this condition maintained the optimal physicochemical properties and the adsorption and removal capacity of thiophene.

Key words: Ce?SBA?15, pH value, Active site, Adsorption desulfurization