Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas

doi:10.1016/j.cjche.2018.06.017

Chinese Journal of Chemical Engineering ›› 2019, Vol. 27 ›› Issue (4): 884-895.DOI: 10.1016/j.cjche.2018.06.017

• Catalysis, Kinetics and Reaction Engineering • Previous Articles Next Articles

Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas

Qian Cheng, Dunyu Liu, Jun Chen, Jing Jin, Wei Li, Shuaishuai Yu

School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China

Received:2018-03-21 Revised:2018-06-10 Online:2019-06-14 Published:2019-04-28
Contact: Dunyu Liu
Supported by:
Supported by the Shanghai Pujiang Program (16PJ1407900).

Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas

Qian Cheng, Dunyu Liu, Jun Chen, Jing Jin, Wei Li, Shuaishuai Yu

School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China

通讯作者: Dunyu Liu
基金资助:
Supported by the Shanghai Pujiang Program (16PJ1407900).

Abstract

Abstract: The removal of NO from oxy-fuel combustion is typically incorporated in sour gas compression purification process. This process involves the oxidation of NO to NO₂ at a high pressure of 1-3 MPa, followed by absorption of NO₂ by water. In this pressure range, the NO conversion rates calculated using the existing kinetic constants are often higher than those obtained experimentally. This study aimed to achieve the regression of kinetic parameters of NO oxidation based on the existing experimental results and theoretical models.
Based on three existing NO oxidation mechanisms, first, the expressions for NO conversion against residence time were derived. By minimizing the mean-square errors of NO conversion ratio, the optimum kinetic rate constants were obtained. Without considering the reverse reaction for NO oxidation, similar mean-square errors for NO conversion ratio were calculated. Considering the reverse reaction for NO oxidation based on the termolecular reaction mechanism, the minimum mean-square error for NO conversion ratio was obtained. Thus, the optimum NO oxidation rate in the pressure range 0.1-3 MPa can be expressed as follows:
-d[NO]/dt=d[NO₂]/dt=0:0026[NO]²[O₂]-0:0034[NO₂]²
Detailed elementary reactions for N₂/NO/NO₂/O₂ system were established to simulate the NO oxidation rate. A sensitivity analysis showed that the critical elementary reaction is 2NO + O₂ ⇌ 2NO₂. However, the simulated NO conversions at a high pressure of 10-30 bar are still higher than the experimental values and similar to those obtained from the models without considering the reverse reaction for NO oxidation.

Key words: Oxy-fuel combustion, NO oxidation, Sour gas compression

摘要： The removal of NO from oxy-fuel combustion is typically incorporated in sour gas compression purification process. This process involves the oxidation of NO to NO₂ at a high pressure of 1-3 MPa, followed by absorption of NO₂ by water. In this pressure range, the NO conversion rates calculated using the existing kinetic constants are often higher than those obtained experimentally. This study aimed to achieve the regression of kinetic parameters of NO oxidation based on the existing experimental results and theoretical models.
Based on three existing NO oxidation mechanisms, first, the expressions for NO conversion against residence time were derived. By minimizing the mean-square errors of NO conversion ratio, the optimum kinetic rate constants were obtained. Without considering the reverse reaction for NO oxidation, similar mean-square errors for NO conversion ratio were calculated. Considering the reverse reaction for NO oxidation based on the termolecular reaction mechanism, the minimum mean-square error for NO conversion ratio was obtained. Thus, the optimum NO oxidation rate in the pressure range 0.1-3 MPa can be expressed as follows:
-d[NO]/dt=d[NO₂]/dt=0:0026[NO]²[O₂]-0:0034[NO₂]²
Detailed elementary reactions for N₂/NO/NO₂/O₂ system were established to simulate the NO oxidation rate. A sensitivity analysis showed that the critical elementary reaction is 2NO + O₂ ⇌ 2NO₂. However, the simulated NO conversions at a high pressure of 10-30 bar are still higher than the experimental values and similar to those obtained from the models without considering the reverse reaction for NO oxidation.

关键词: Oxy-fuel combustion, NO oxidation, Sour gas compression

Qian Cheng, Dunyu Liu, Jun Chen, Jing Jin, Wei Li, Shuaishuai Yu. Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas[J]. Chinese Journal of Chemical Engineering, 2019, 27(4): 884-895.

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Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas

Gas-phase oxidation of NO at high pressure relevant to sour gas compression purification process for oxy-fuel combustion flue gas

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