同位素交换技术测定氮气在N<sub>2</sub>–CO<sub>2</sub>–CO–Ar与铁液界面的反应速率常数

陈中子; 范越文; 胡晓军; 周国治

doi:10.1007/s12613-025-3319-z

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Zhongzi Chen, Yuewen Fan, Xiaojun Hu, and Kuochih Chou, Determination of interfacial reaction rate constant of nitrogen between N₂–CO₂–CO–Ar and molten iron using isotope exchange technique, Int. J. Miner. Metall. Mater., (2026). https://doi.org/10.1007/s12613-025-3319-z

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同位素交换技术测定氮气在N₂–CO₂–CO–Ar与铁液界面的反应速率常数

摘要: 在低碳冶金背景下，CO₂炼钢技术被认为是一种具有潜力的碳循环利用途径，但在此气氛条件下N₂在气液界面的反应动力学仍缺乏系统研究。本文采用同位素交换技术，研究了N₂–CO₂–CO–Ar气氛与液态铁之间的界面反应行为。在1873 K下，通过在线质谱实时监测气相中²⁸N₂、²⁹N₂和³⁰N₂的变化，计算得到N₂的界面反应速率常数(k_c)。针对不同的CO₂/CO比例计算了相关动力学参数，实验结果表明，使用CO₂–CO气氛调控氧势的条件下，界面反应速率常数约为4.35 × 10⁻⁶ mol·m⁻²·s⁻¹·Pa⁻¹。依据实验数据分析得出，铁液中的O、C、S对氮溶解起到了抑制作用。并且建立模型获得了三种元素在液态铁表面的吸附系数，以确定界面反应速率常数与铁液中O、C、S活度之间的定量关系： \textk_\textc\text=\frac\text4.35×10^-6\left(\text1+14.25\texta_\textO\text+0.25\texta_\textC\text+6.50\texta_\textS\right)^2 。该研究为CO₂炼钢条件下氮溶解的动力学研究提供了重要基础数据和理论依据。

Determination of interfacial reaction rate constant of nitrogen between N₂–CO₂–CO–Ar and molten iron using isotope exchange technique

Abstract: The application of CO₂ in the steelmaking process has yielded promising results, demonstrating a certain capability for nitrogen removal. To accurately determine the kinetic parameters of nitrogen reactions at the iron melt interface under CO₂ injection conditions, an isotope exchange technique was employed. This technique was used to monitor the evolution of the nitrogen isotopic composition during the reaction between a ²⁸N₂–³⁰N₂–CO₂–CO–Ar gas mixture and an iron melt of controlled composition. The kinetic parameters of nitrogen were subsequently calculated for various CO₂/CO ratios. Furthermore, the dissociation rate determining model was applied to establish the relationship between the interfacial reaction rate constant (k_c) and the activity of surfactive elements (O, C, and S) in molten iron (a_O, a_C, and a_S), expressed as k_\rm c=\dfrac4.35\times10^-6\left(1+14.25a_\rm O+0.25a_\rm C+6.50a_\rm S\right)^2 .

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同位素交换技术测定氮气在N2–CO2–CO–Ar与铁液界面的反应速率常数

Determination of interfacial reaction rate constant of nitrogen between N2–CO2–CO–Ar and molten iron using isotope exchange technique

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同位素交换技术测定氮气在N₂–CO₂–CO–Ar与铁液界面的反应速率常数

Determination of interfacial reaction rate constant of nitrogen between N₂–CO₂–CO–Ar and molten iron using isotope exchange technique