基于IMCT理论的CaO-SiO2-MgO-Al2O3-FeO-P2O5-TiO2渣系脱磷热力学模型

刘然; 刘晏廷; 高艳甲; 兰臣臣; 闫光石; 吕庆

doi:10.7513/j.issn.1004-7638.2024.04.016

基于IMCT理论的CaO-SiO₂-MgO-Al₂O₃-FeO-P₂O₅-TiO₂渣系脱磷热力学模型

doi: 10.7513/j.issn.1004-7638.2024.04.016

刘然^1,,
刘晏廷¹,
高艳甲^{1, 2},
兰臣臣¹,
闫光石¹,
吕庆¹

1.
华北理工大学冶金与能源学院, 河北唐山 063000
2.
承德钢铁集团有限公司, 河北承德 067102

基金项目: 国家自然科学基金项目(52204344)；承德市科技计划项目（202205B060）；华北理工大学研究生创新项目（2023B05）。

详细信息

作者简介:
刘然，1979年出生，男，河北衡水人，博士，教授，主要研究方向为冶金智能化与非高炉炼铁，E-mail：liuran@ncst.edu.cn

中图分类号: TF55
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出版历程
- 收稿日期: 2023-10-31
- 刊出日期: 2024-08-30

Thermodynamic model of dephosphorization of CaO-SiO₂-MgO-Al₂O₃-FeO-P₂O₅-TiO₂ slag system based on IMCT theory

1.
College of Metallurgy and Energy, North China University of Science and Technology, Tangshan 063000, Hebei, China
2.
Chengde Iron and Steel Group Co., Ltd., Chengde 067102, Hebei, China

摘要

摘要: 基于离子分子共存理论（IMCT）建立了CaO-SiO₂-MgO-Al₂O₃-FeO-P₂O₅-TiO₂七元熔渣磷分配比(L_P)模型，该模型已在多个熔渣体系中被验证，具有较为精确的预测磷富集行为的能力，进一步分析了各组元成分对活度及L_P的影响，通过该模型总结了冶炼钒钛磁铁矿的合理熔渣成分。结果表明：在1000～1600 ℃范围内，随着温度的升高，FeO、MgO与CaO活度上升，SiO₂与Al₂O₃的活度随之减小，对TiO₂无明显影响。随着碱度由0.92升高至1.32，CaO、MgO的活度明显上升，SiO₂和Al₂O₃的活度明显下降，FeO的活度逐渐增加，TiO₂的活度基本保持不变。随着渣中CaO质量分数增加，Al₂O₃、SiO₂的活度随之减少，CaO、MgO、FeO的活度随之增大。随着渣中SiO₂质量分数增加，渣中碱性氧化物CaO、MgO、FeO的活度随之减少，渣中酸性氧化物SiO₂、Al₂O₃、SiO₂的活度随之增加。渣系中MgO质量分数由4%增加到14.5%后，各组元活度的变化规律与CaO基本相同，但影响程度弱于CaO。渣系中Al₂O₃、FeO和TiO₂质量分数增加后，仅使得自身活度显著增加，对其它组元的活度影响程度相对较小；随着碱度和FeO质量分数的增加，L_P逐渐增加；随着MgO质量分数的增加，L_p先降低后增加；随Al₂O₃、TiO₂质量分数的增加，L_P逐渐降低；TiO₂质量分数在10%左右时，选取熔渣组分为CaO(35.5%)-SiO₂(26%)-MgO(10.2%)-Al₂O₃(12.5%)-FeO(5%)- TiO₂，铁水中[P]可控制在0.01%以下。
- 钒钛磁铁矿 /
- HIsmelt工艺 /
- 熔渣 /
- 磷分配比 /
- 热力学模型 /
- 离子分子共存理论
Abstract: Based on the theory of ionic-molecular coexistence (IMCT), a seven-component slag phosphorus distribution ratio (L_P) model for CaO-SiO₂-MgO-Al₂O₃-FeO-P₂O₅-TiO₂ was established. This model has been validated in multiple slag systems and has the ability to accurately predict the enrichment behavior of phosphorus. The influence of each component on activity and L_P was further analyzed, and the reasonable slag composition for smelting vanadium-titanium magnetite was summarized through this model. The results show that within the temperature range of 1000 to 1600 °C, as the temperature increases, the activities of FeO, MgO and CaO increase, while those of SiO₂ and Al₂O₃ decrease, with no significant effect on TiO₂. As the basicity increases from 0.92 to 1.32, the activities of CaO and MgO significantly increase, while those of SiO₂ and Al₂O₃ decrease significantly, with a gradual increase in the activity of FeO and a nearly constant activity of TiO₂. As the mass fraction of CaO in the slag increases, the activities of Al₂O₃ and SiO₂ decrease, while those of CaO, MgO and FeO increase. As the mass fraction of SiO₂ in the slag increases, the activities of basic oxides CaO, MgO and FeO decrease, while those of acidic oxides SiO₂, Al₂O₃ and TiO₂ increase. After increasing the mass fraction of MgO in the slag from 4% to 14.5%, the variation law of each component activity is basically the same as that of CaO, but the influence is weaker than that of CaO. After increasing the mass fraction of Al₂O₃, FeO and TiO₂ in the slag, only their own activities significantly increase, with relatively small effects on the activities of other components. As the basicity and FeO mass fraction increase, L_P gradually increases. As the MgO mass fraction increases, L_p first decreases and then increases. As the Al₂O₃ and TiO₂ mass fractions increase, L_P gradually decreases. When the TiO₂ mass fraction is around 10%, the slag composition of CaO (35.5%)-SiO₂ (26%)-MgO (10.2%)-Al₂O₃ (12.5%)-FeO (5%)-TiO₂ is selected, and the [P] in the molten iron can be controlled below 0.01%.
- vanadium titanium magnetite /
- HIsmelt process /
- slag /
- phosphorus ratio /
- thermodynamic model /
- ion and molecule coexistence theory

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图 1 炉渣组元活度与温度的关系

Figure 1. Relationship between the activity of slag components and temperature

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图 2 炉渣组元活度与碱度的关系

Figure 2. Relationship between activity and alkalinity of slag components

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图 3 炉渣组元活度与炉渣成分的关系

（a）CaO质量分数与各组元活度的关系；（b）SiO₂质量分数与各组元活度的关系；（c）MgO质量分数与各组元活度的关系；（d）Al₂O₃质量分数与各组元活度的关系；（e）FeO质量分数与各组元活度的关系；（f）TiO₂质量分数与各组元活度的关系

Figure 3. Relationship between activity of slag components and slag composition

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图 4 七元渣系组元质量百分数与磷分配比的关系

(a)CaO/SiO₂与磷分配比的关系；(b)MgO与磷分配比的关系；(c)Al₂O₃与磷分配比的关系；(d)TiO₂与磷分配比的关系；(e)FeO与磷分配比的关系

Figure 4. Relationship between mass percentage of slag components and L_P

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表 1 炉渣界面脱磷反应的标准吉布斯自由能和自由常数

Table 1. Standard Gibbs free energy and free constant of slag interface dephosphorization reaction

炉渣界面脱磷反应	$ \Delta_{\text{r}}G_{^{\text{m}}}^{\mathrm{\theta}}/\left(\text{J}\cdot\text{mo}\text{l}^{-1}\right) $	$ K_{\text{c}i}^{\theta} $
$ {\text{5(Fe}}_{\text{t}}^{{\text{2}}+} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = {{{\mathrm{P}}_2 {\mathrm{O}}_5}} + {\text{5tFe}} $	$ - 122\;412 + 312.522 T $	$ K_{{{{\mathrm{P}}_2 {\mathrm{O}}_5}}}^{\theta} = \dfrac{{{N_{{\mathrm{P}}_2 {\mathrm{O}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{\rm{{Fe_t}O}}^5 a_{\left[ {\text{P}} \right]}^2}} $
$ {\text{2(C}}{{\text{a}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{2CaO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 680\;599 + 330.552 T $	$ K_{2\text{CaO}\cdot\mathrm{P}_2\mathrm{O}_5}^{\theta}=\dfrac{N_{2\text{CaO}\cdot\mathrm{P}_2\mathrm{O}_5}a_{\text{Fe}}^{5\text{t}}}{N_{\text{CaO}}^2N_{{{\mathrm{Fe}}_{\mathrm{t}}{\mathrm{O}}}}^5a_{\left[\text{P}\right]}^2} $
$ {\text{3(C}}{{\text{a}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{3CaO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 805\;282 + 301.264 T $	$ K_{3{\text{CaO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}^{\theta} = \dfrac{{{N_{3{\text{CaO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{{\text{CaO}}}^3 N_{\rm{{Fe_t}O}}^5 a_{\left[ {\text{P}} \right]}^2}} $
$ {\text{4(C}}{{\text{a}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{4CaO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 565\;964 + 291.641 T $	$ K_{4{\text{CaO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}^{\theta} = \dfrac{{{N_{4{\text{CaO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{{\text{CaO}}}^4 N_{\rm{{Fe_t}O}}^5 a_{\left[ {\text{P}} \right]}^2}} $
$ {\text{2(M}}{{\text{g}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{2MgO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ 72\;977 - 44.243 T $	$ K_{2{\text{MgO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}^{\theta} = \dfrac{{{N_{2{\text{MgO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{{\text{MgO}}}^2 N_{\rm{{Fe_t}O}}^5 a_{\left[ {\text{P}} \right]}^2}} $
$ {\text{3(M}}{{\text{g}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{3MgO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 484\;369 + 254.831 T $	$ K_{3{\text{MgO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}^{\theta} = \dfrac{{{N_{3{\text{MgO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{{\text{MgO}}}^3 N_{\rm{{Fe_t}O}}^5 a_{\left[ {\text{P}} \right]}^2}} $
$ {\text{5(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{3(F}}{{\text{e}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{3FeO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 525\;769 + 387.822 T $	$ K_{3\text{FeO}\cdot\mathrm{P}_2\mathrm{O}_5}^{{\theta}}=\dfrac{N_{3\text{FeO}\cdot\mathrm{P}_2\mathrm{O}_5}a_{\text{Fe}}^{5\text{t}}}{N_{\mathrm{Fe}_{\mathrm{t}}\mathrm{O}}^5N_{\text{FeO}}^3a_{\left[\text{P}\right]}^2} $
$ {\text{(Fe}}_{\text{t}}^{{\text{2}} + } + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{4(F}}{{\text{e}}^{{\text{2}} + }} + {{\text{O}}^{{\text{2}} - }}{\text{)}} + {\text{2}}\left[ {\text{P}} \right] = \left( {{\text{4FeO}} \cdot {\mathrm{P}}_2 {\mathrm{O}}_5} \right) + {\text{5tFe}} $	$ - 477\;223 + 342.481 T $	$ K_{4{\text{FeO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}^{\theta} = \dfrac{{{N_{4{\text{FeO}} \cdot {{{\mathrm{P}}_2 {\mathrm{O}}}}_5}}a_{{\text{Fe}}}^{5{\text{t}}}}}{{N_{\rm{{Fe_t}O}}^5 N_{{\text{FeO}}}^4 a_{\left[ {\text{P}} \right]}^2}} $

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表 2 高磷钒钛矿炉渣最佳炉渣成分计算

Table 2. The optimal slag compositions of high phosphorus vanadium titanium ore slag %

	TiO₂	CaO	SiO₂	MgO	Al₂O₃	FeO
模型预测	10.5	35.5	26	10.2	12.5	5
60%钒钛磁铁矿^[6]	9.92	33.26	26.6	7.43	12.97	6.85

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