Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

doi:10.1016/j.cjche.2024.10.022

Chinese Journal of Chemical Engineering ›› 2025, Vol. 78 ›› Issue (2): 232-244.DOI: 10.1016/j.cjche.2024.10.022

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Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

Feng Gao^1,2,3, Sixiao Zhu^1,2,3, Liping Chang^1,2,3, Weiren Bao^1,2,3, Jinghong Ma^3,4, Junjie Liao^1,2,3,4

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China;
3. School of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China;
4. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030024, China

Received:2024-07-08 Revised:2024-10-18 Accepted:2024-10-20 Online:2024-12-06 Published:2025-02-08
Supported by:
The authors gratefully acknowledge the financial support of Ningbo Fareast Tech Catalyst Engineering Co., Ltd, the National Natural Science Foundation of China (22478275), Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2022SX–TD014).

Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

Feng Gao^1,2,3, Sixiao Zhu^1,2,3, Liping Chang^1,2,3, Weiren Bao^1,2,3, Jinghong Ma^3,4, Junjie Liao^1,2,3,4

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China;
3. School of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China;
4. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030024, China

通讯作者: Junjie Liao,E-mail:liaojunjie@tyut.edu.cn
基金资助:
The authors gratefully acknowledge the financial support of Ningbo Fareast Tech Catalyst Engineering Co., Ltd, the National Natural Science Foundation of China (22478275), Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2022SX–TD014).

Abstract

Abstract: The removal of H₂S from coke oven gas (COG) is an important issue for the further utilization of COG. Zeolites could be used for industrial desulfurization owing to their high thermal stability and regenerability. However, further analysis on the kinetics of deep desulfurization using zeolites is necessary to provide relevant information for industrial design. In this study, the desulfurization breakthrough curves of faujasite (FAU) zeolite in COG were measured using a fixed bed reactor. The adsorption isotherm was investigated using the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich models. The adsorption saturated capacity of H₂S was inversely related to the temperature. The results show that the Langmuir model best fits the adsorption isotherm with a lower value of root-mean-square-error (RMSE) and Chi-Square (χ²), and the calculated activation energy is 14.62 kJ·mol^-1. The adsorption kinetics were investigated using pseudo-first-order (PFO), pseudo-second-order (PSO), Bangham and Weber-Morris models. The Bangham model fitted the kinetic data well, indicating that pore diffusion is an influential factor in the adsorption process. The Weber-Morris model suggests that the adsorption rate was not solely determined by the pore diffusion, but was also influenced by the active site on the FAU zeolite. The adsorption breakthrough curves under different gas flow rates were fitted using the bed depth service time (BDST) model, and it provides an accurate prediction of the breakthrough time with a small relative error. The results of thermodynamic analysis demonstrated the feasibility and spontaneity (ΔG<0) and exothermic (ΔH<0) nature of the adsorption process of the FAU zeolite for H₂S under COG.

Key words: H₂S, Coke oven gas, FAU zeolite, Kinetics, Adsorption, Fixed-bed

摘要： The removal of H₂S from coke oven gas (COG) is an important issue for the further utilization of COG. Zeolites could be used for industrial desulfurization owing to their high thermal stability and regenerability. However, further analysis on the kinetics of deep desulfurization using zeolites is necessary to provide relevant information for industrial design. In this study, the desulfurization breakthrough curves of faujasite (FAU) zeolite in COG were measured using a fixed bed reactor. The adsorption isotherm was investigated using the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich models. The adsorption saturated capacity of H₂S was inversely related to the temperature. The results show that the Langmuir model best fits the adsorption isotherm with a lower value of root-mean-square-error (RMSE) and Chi-Square (χ²), and the calculated activation energy is 14.62 kJ·mol^-1. The adsorption kinetics were investigated using pseudo-first-order (PFO), pseudo-second-order (PSO), Bangham and Weber-Morris models. The Bangham model fitted the kinetic data well, indicating that pore diffusion is an influential factor in the adsorption process. The Weber-Morris model suggests that the adsorption rate was not solely determined by the pore diffusion, but was also influenced by the active site on the FAU zeolite. The adsorption breakthrough curves under different gas flow rates were fitted using the bed depth service time (BDST) model, and it provides an accurate prediction of the breakthrough time with a small relative error. The results of thermodynamic analysis demonstrated the feasibility and spontaneity (ΔG<0) and exothermic (ΔH<0) nature of the adsorption process of the FAU zeolite for H₂S under COG.

关键词: H₂S, Coke oven gas, FAU zeolite, Kinetics, Adsorption, Fixed-bed

Feng Gao, Sixiao Zhu, Liping Chang, Weiren Bao, Jinghong Ma, Junjie Liao. Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies[J]. Chinese Journal of Chemical Engineering, 2025, 78(2): 232-244.

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Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

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