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

doi:10.1016/j.cjche.2022.07.002

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. 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. 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

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

Chao Yang, Zhelin Su, Yeshuang Wang, Huiling Fan, Meisheng Liang, Zhaohui Chen. Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO₂ adsorbents[J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 233-241.

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

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

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