SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2023, Vol. 56 ›› Issue (4): 233-241.DOI: 10.1016/j.cjche.2022.07.002

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Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO2 adsorbents

Chao Yang1, Zhelin Su2, Yeshuang Wang2, Huiling Fan2, Meisheng Liang1, Zhaohui Chen3   

  1. 1. College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China;
    2. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
    3. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
  • Received:2022-03-23 Revised:2022-06-30 Online:2023-06-13 Published:2023-04-28
  • Contact: Huiling Fan,E-mail:fanhuiling@tyut.edu.cn;Zhaohui Chen,E-mail:zhhchen@ipe.ac.cn
  • Supported by:
    This work is financially supported by the National Natural Science Foundation of China (22078223 and 21878209) and Shanxi Province Science Foundation for Youths (20210302123065).

Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO2 adsorbents

Chao Yang1, Zhelin Su2, Yeshuang Wang2, Huiling Fan2, Meisheng Liang1, Zhaohui Chen3   

  1. 1. College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China;
    2. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
    3. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
  • 通讯作者: Huiling Fan,E-mail:fanhuiling@tyut.edu.cn;Zhaohui Chen,E-mail:zhhchen@ipe.ac.cn
  • 基金资助:
    This work is financially supported by the National Natural Science Foundation of China (22078223 and 21878209) and Shanxi Province Science Foundation for Youths (20210302123065).

Abstract: A series of ZnO/SiO2 adsorbents were prepared by a sol–gel method using tetraethyl orthosilicate, ethylene glycol (EG) and nitrates as precursors. The effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in detail. It is found that the low drying temperature led to a weak interaction among EG, SiOH/H2O and the nitrates in the gel system, which caused the oxidation of EG by NO3- and formed zinc glyoxylate complex during the gel calcination process, whereas this oxidation process also occurred at a high drying temperature during the gel drying process. The formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of ZnO, which resulted in the inferior desulfurization performance of adsorbents despite they have smaller ZnO nanoparticles. The gel dried at 120 ℃ formed the hydrogen bonds between EG and SiOH/H2O and a strong interaction between zinc oxo-clusters and NO3- was also found in the gel system, which avoided the oxidation of EG by NO3- during the preparation process and the ZnO nanoparticles with sizes of 6 nm were formed by a combustion method. The adsorbent affords a highest sulfur capacity of 104.9 mg·g-1 in this case. In addition, the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area.

Key words: Sol–gel method, Drying temperature, H2S removal, Zinc–silica composites, Hydrogen bonds

摘要: A series of ZnO/SiO2 adsorbents were prepared by a sol–gel method using tetraethyl orthosilicate, ethylene glycol (EG) and nitrates as precursors. The effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in detail. It is found that the low drying temperature led to a weak interaction among EG, SiOH/H2O and the nitrates in the gel system, which caused the oxidation of EG by NO3- and formed zinc glyoxylate complex during the gel calcination process, whereas this oxidation process also occurred at a high drying temperature during the gel drying process. The formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of ZnO, which resulted in the inferior desulfurization performance of adsorbents despite they have smaller ZnO nanoparticles. The gel dried at 120 ℃ formed the hydrogen bonds between EG and SiOH/H2O and a strong interaction between zinc oxo-clusters and NO3- was also found in the gel system, which avoided the oxidation of EG by NO3- during the preparation process and the ZnO nanoparticles with sizes of 6 nm were formed by a combustion method. The adsorbent affords a highest sulfur capacity of 104.9 mg·g-1 in this case. In addition, the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area.

关键词: Sol–gel method, Drying temperature, H2S removal, Zinc–silica composites, Hydrogen bonds