N2-CO-CO2-H2O气氛下K(g)对焦炭高温气化反应动力学的影响

doi:10.13228/j.boyuan.issn1006-9356.20220177

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摘要为了掌握高温区碱金属对焦炭气化过程的影响,在N₂-CO-CO₂-H₂O和N₂-CO-CO₂-H₂O-K_(g)气氛下,利用热失重法分别研究了焦炭在1 413~1 773 K的气化反应特征。结果显示,K_(g)对焦炭的气化反应具有较强的正催化作用,可以显著提高有效内扩散系数(D_e)和界面反应速率常数(k₊),降低内扩散活化能与界面反应活化能,且K_(g)对内扩散的影响程度高于对界面反应的影响。随着反应率的增加,内扩散阻力(η_i)和界面反应阻力(η_C)均逐渐增加,K_(g)可以促进η_i和η_C降低。在N₂-CO-CO₂-H₂O气氛、1 413 K时,气化反应的限制性环节逐渐由界面反应转为内扩散;而在1 473、1 573、1 673和1 773 K时其限制性环节始终为界面反应。在N₂-CO-CO₂-H₂O-K_(g)气氛下,气化反应的限制性环节始终为界面反应。

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关键词 ：焦炭, 气化, K_(g), 反应阻力, 限制性环节

Abstract：In order to understand the influence of alkali metals in high temperature zone on coke gasification process, the kinetic behaviors of coke gasification in the temperature 1 413-1 773 K were studied by thermogravimetric analysis under atmospheres of N₂-CO-CO₂-H₂O and N₂-CO-CO₂-H₂O-K_(g). The results show that K_(g) has a strong positive catalytic effect on the gasification reaction of coke, which can significantly improve the effective internal diffusion coefficient (D_e) and interfacial reaction rate constant (k₊), reduce the activation energy of internal diffusion and interfacial reaction, and the influence of K_(g) on internal diffusion is higher than that on interfacial reaction. With increase of reaction rate, the internal diffusion resistance (η_i) and interfacial reaction resistance (η_C) increase gradually, whereas K_(g) tends to decrease η_i and η_C. Under the N₂-CO-CO₂-H₂O atmosphere at 1 413 K, the controlling factor gradually changes from interfacial reaction to internal diffusion. At 1 473, 1 573, 1 673 and 1 773 K, the controlling factor is always interface reaction. Under the N₂-CO-CO₂-H₂O-K_(g) atmosphere, the controlling factor is the interface reaction.

Key words： coke gasification K_(g) reaction resistance controlling factor

收稿日期: 2022-02-24

基金资助:河北省自然科学基金资助项目(E2021209046, E2019209424, E2020209208); 唐山市科技计划资助项目(21130209C); 河北省省属高等学校基本科研业务费资助项目(JQN2021015)

通讯作者: 刘然(1979—), 男, 博士, 教授; E-mail: liuran@ncst.edu.cn

作者简介: 兰臣臣(1989—), 男, 博士, 讲师; E-mail: 15081586028@163.com

引用本文:

兰臣臣, 张淑会, 刘然, 吕庆, 李福民. N₂-CO-CO₂-H₂O气氛下K_(g)对焦炭高温气化反应动力学的影响[J]. 中国冶金, 2022, 32(7): 12-19. LAN Chen-chen, ZHANG Shu-hui, LIU Ran, LÜ Qing, LI Fu-min. Effect of K_(g) on high temperature gasification kinetics of coke in N₂-CO-CO₂-H₂O atmosphere[J]. China Metallurgy, 2022, 32(7): 12-19.

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http://www.zgyj.ac.cn/CN/10.13228/j.boyuan.issn1006-9356.20220177 或 http://www.zgyj.ac.cn/CN/Y2022/V32/I7/12

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