重金属短流程冶金炉渣活度研究与过程数值模拟
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摘要
短流程清洁冶金是重金属冶金技术的发展方向。近几十年来,国内外先后出现了多种短流程直接炼铅和连续炼铜试验方案,有的已经实现了工业化。但是,短流程清洁冶金无论在工艺流程,还是在基础理论上,仍有不少问题有待研究解决。
本论文以“闪速炼铅”和“闪速连续炼铜”为研究对象,通过开展新型冶金炉渣活度研究和过程数值模拟,探索重金属短流程冶金规律,以完善直接炼铅和连续炼铜理论,为其工业应用提供理论依据和实践指导,促进该项具有自主知识产权的重金属短流程冶金新技术的发展。论文的主要研究内容如下：
基于炉渣结构共存理论,研究建立了Cu2O-CaO-Fe2O3三元渣系、Cu20-CaO-SiO2-FeO-Fe2O3五元渣系和PbO-ZnO-CaO-SiO2-FeO-Fe2O3六元渣系的组元活度计算模型,计算并绘制了渣中CaO、Cu2O、Fe2O3、PbO和ZnO等组元的等活度曲线图,考察了碱度和温度等因素对组元活度NCaO、NCu2O、NFe2O3和组元活度系数γCu2O、γFeO、γPbO、γZnO的影响。结果表明,计算值与文献实测值吻合程度高,模型能较好地反映炉渣体系的结构本质；研究结果填补了新型冶金炉渣的活度数据,也证明了炉渣结构共存理论用于有色冶金领域的可行性。
基于最小吉布斯自由能原理,研究建立了闪速炼铅过程多相平衡数学模型；基于此模型,对闪速炼铅过程进行了多因素耦合仿真,通过改变吨矿氧量(OVPTC)、富氧浓度(OG)、熔炼温度(T)、熔剂量以及精矿成分,研究了各工艺参数对粗铅含硫、烟尘率、熔炼直收率的综合影响,研究了闪速炼铅过程的相组成变化规律和氧(硫)势变化情况,研究了铅、锌、铜、铁在闪速炼铅各相中的分配行为。结果表明,所建立模型的模拟结果与奥托昆普半工业试验数据吻合的较好,能较好地反映闪速炼铅实际；奥托昆普公司采用122 Nm3/t的富氧(OG=95%)在1210℃进行闪速炼铅半工业试验,是综合考虑粗铅含硫、烟尘率及铅的直收率等因素的结果。
将闪速连续炼铜过程视为由相对独立的闪速造锍熔炼过程和连续吹炼造铜过程构成,分别建立了闪速造锍熔炼多相平衡数学模型和连续吹炼造铜局域平衡数学模型,并通过中间物料的传递将两模型有机结合,从而构建了完整的闪速连续炼铜过程数学模型。基于此模型,对闪速连续炼铜过程进行了多因素耦合仿真,研究了炉型结构、炉渣渣型和铜锍品位对闪速连续炼铜过程粗铜生成热力学的影响；研究了闪速连续炼铜过程的相组成变化规律和氧(硫)势变化情况；研究了吨矿氧量(OVPTC)、富氧浓度(OG)、熔炼温度(T)和精矿组成等工艺参数对粗铜含硫、Fe3O4行为、渣含铜、熔炼直收率,以及铁、铜锍在闪速连续炼铜过程中行为的综合影响。结果表明,甩渣吹炼的双烟道闪速连续炼铜炉是比较理想的连续炼铜炉体；在该炉中进行闪速连续炼铜时,熔炼直收率可达97%以上。
Short-flow clean smelting process is the development direction of heavy metal metallurgical technology. There have appeared some pilot programs of lead direct smelting and copper continuous smelting in the world in the past several decades, and some of them have already industrialized. But, no matter the smelting process or the metallurgical theory of the short-flow clean smelting, there are still many issues to be solve.
In this paper, the slag activity research and the numerical simulation of the "lead flash smelting process" and "copper flash continuous smelting process", which have the independent intellectual property rights of china, were finished by the author. Those researches are helpful to explore the metallurgical law of those short-flow clean smelting processes, to perfect the theories of lead direct smelting and copper continuous smelting, to provide theoretical basis and practical guidance for the industrial applications of them, and also, to promote the development of those technologies. The specific research are shown as follows:
According to the coexistence theory of slag structure, the activity calculation models for slag system of CaO-Cu2O-Fe2O3, Cu2O-CaO-SiO2-FeO-Fe2O3 and PbO-ZnO-CaO-SiO2-FeO-Fe2O3 were built. Then, the equal activity curves of CaO、Cu2O、Fe2O3、PbO and ZnO in those slag were drawed, and the influences of basicity and temperature on the activities NcaO、Ncu2O、NFe2O3 and the activity coefficientsγCu2o、γFeO、γPbO、γZnO were also analyzed. Results show that the calculated values are in good agreement with the reported measured values, showing that those models can wholly embody those slag structural characteristics. The research results supplemented the activity data of those new metallurgical slags, and proved the feasibility for the coexistence theory of slag structure to be applied to the field of non-ferrous metallurgy.
Based on the principle of Gibbs free energy minimization, the thermodynamic model of the lead flash smelting process was built. Then, the multi-factor coupled simulation of the lead flash smelting process was carried out based on the model. By adjusting the Oxygen Volume Per Ton Concentrate (OVPTC), Oxygen Grade (OG), Temperature (T), flux quantity and concentrate composition, the integrated influences of those technology parameters on the sulfur content in bullion, the dust rate and the recovery rate of Pb were analyzed, and the change trends of equilibrium phase composition, oxygen potential and sulfur potential were studied, and the distribution behavior of Pb, Zn, Cu and Fe in each phase were also investigated. Results show that the thermodynamic model calculated values are in good agreement with the Outokumpu semi-industrial test values, and the model can wholly embody the lead flash smelting practice. It's a deliberate result for Outokumpu company, by taking into account the sulfur content in bullion, the dust rate, the recovery rate of Pb and so on, to carry out semi-industrial pilot, while OVPTC is 122 Nm3/t, OG is 95% and smelting temperature is 1210℃.
The copper flash continuous smelting furnace can be regarded as a synthesis reactor of two relatively independent processes:Flash Matting Smelting Process (FMSP) and Copper Continuous Converting Process (CCCP). Based on this thinking, the multi-phase equilibrium model of FMSP and the local-equilibrium model of CCCP were built, and the integrated model of the copper flash continuous smelting process was made up by combinating the above two models with smelting intermediate materials. Then, the multi-factor coupled simulation of the copper flash continuous smelting process was carried out based on the integrated model. The influences of furnace structure, slag type and matte grade on blister formation thermodynamic condition were analyzed, and the change trends of equilibrium phase composition, oxygen potential and sulfur potential were studied, and the integrated influences of the technology parameters, including the Oxygen Volume Per Ton Concentrate (OVPTC), Oxygen Grade (OG), Temperature (T) and concentrate composition, on the sulfur content in blister, Fe3O4 behavior, copper content in slag, recovery rate of Cu, the behavior of Fe and matte were also investigated. Results show that the flash furnace, with double flues and slag partition wall, is an ideal reactor for copper flash continuous smelting, and the recovery rate of copper can be more than 97%.
本论文以“闪速炼铅”和“闪速连续炼铜”为研究对象,通过开展新型冶金炉渣活度研究和过程数值模拟,探索重金属短流程冶金规律,以完善直接炼铅和连续炼铜理论,为其工业应用提供理论依据和实践指导,促进该项具有自主知识产权的重金属短流程冶金新技术的发展。论文的主要研究内容如下：
基于炉渣结构共存理论,研究建立了Cu2O-CaO-Fe2O3三元渣系、Cu20-CaO-SiO2-FeO-Fe2O3五元渣系和PbO-ZnO-CaO-SiO2-FeO-Fe2O3六元渣系的组元活度计算模型,计算并绘制了渣中CaO、Cu2O、Fe2O3、PbO和ZnO等组元的等活度曲线图,考察了碱度和温度等因素对组元活度NCaO、NCu2O、NFe2O3和组元活度系数γCu2O、γFeO、γPbO、γZnO的影响。结果表明,计算值与文献实测值吻合程度高,模型能较好地反映炉渣体系的结构本质；研究结果填补了新型冶金炉渣的活度数据,也证明了炉渣结构共存理论用于有色冶金领域的可行性。
基于最小吉布斯自由能原理,研究建立了闪速炼铅过程多相平衡数学模型；基于此模型,对闪速炼铅过程进行了多因素耦合仿真,通过改变吨矿氧量(OVPTC)、富氧浓度(OG)、熔炼温度(T)、熔剂量以及精矿成分,研究了各工艺参数对粗铅含硫、烟尘率、熔炼直收率的综合影响,研究了闪速炼铅过程的相组成变化规律和氧(硫)势变化情况,研究了铅、锌、铜、铁在闪速炼铅各相中的分配行为。结果表明,所建立模型的模拟结果与奥托昆普半工业试验数据吻合的较好,能较好地反映闪速炼铅实际；奥托昆普公司采用122 Nm3/t的富氧(OG=95%)在1210℃进行闪速炼铅半工业试验,是综合考虑粗铅含硫、烟尘率及铅的直收率等因素的结果。
将闪速连续炼铜过程视为由相对独立的闪速造锍熔炼过程和连续吹炼造铜过程构成,分别建立了闪速造锍熔炼多相平衡数学模型和连续吹炼造铜局域平衡数学模型,并通过中间物料的传递将两模型有机结合,从而构建了完整的闪速连续炼铜过程数学模型。基于此模型,对闪速连续炼铜过程进行了多因素耦合仿真,研究了炉型结构、炉渣渣型和铜锍品位对闪速连续炼铜过程粗铜生成热力学的影响；研究了闪速连续炼铜过程的相组成变化规律和氧(硫)势变化情况；研究了吨矿氧量(OVPTC)、富氧浓度(OG)、熔炼温度(T)和精矿组成等工艺参数对粗铜含硫、Fe3O4行为、渣含铜、熔炼直收率,以及铁、铜锍在闪速连续炼铜过程中行为的综合影响。结果表明,甩渣吹炼的双烟道闪速连续炼铜炉是比较理想的连续炼铜炉体；在该炉中进行闪速连续炼铜时,熔炼直收率可达97%以上。
Short-flow clean smelting process is the development direction of heavy metal metallurgical technology. There have appeared some pilot programs of lead direct smelting and copper continuous smelting in the world in the past several decades, and some of them have already industrialized. But, no matter the smelting process or the metallurgical theory of the short-flow clean smelting, there are still many issues to be solve.
In this paper, the slag activity research and the numerical simulation of the "lead flash smelting process" and "copper flash continuous smelting process", which have the independent intellectual property rights of china, were finished by the author. Those researches are helpful to explore the metallurgical law of those short-flow clean smelting processes, to perfect the theories of lead direct smelting and copper continuous smelting, to provide theoretical basis and practical guidance for the industrial applications of them, and also, to promote the development of those technologies. The specific research are shown as follows:
According to the coexistence theory of slag structure, the activity calculation models for slag system of CaO-Cu2O-Fe2O3, Cu2O-CaO-SiO2-FeO-Fe2O3 and PbO-ZnO-CaO-SiO2-FeO-Fe2O3 were built. Then, the equal activity curves of CaO、Cu2O、Fe2O3、PbO and ZnO in those slag were drawed, and the influences of basicity and temperature on the activities NcaO、Ncu2O、NFe2O3 and the activity coefficientsγCu2o、γFeO、γPbO、γZnO were also analyzed. Results show that the calculated values are in good agreement with the reported measured values, showing that those models can wholly embody those slag structural characteristics. The research results supplemented the activity data of those new metallurgical slags, and proved the feasibility for the coexistence theory of slag structure to be applied to the field of non-ferrous metallurgy.
Based on the principle of Gibbs free energy minimization, the thermodynamic model of the lead flash smelting process was built. Then, the multi-factor coupled simulation of the lead flash smelting process was carried out based on the model. By adjusting the Oxygen Volume Per Ton Concentrate (OVPTC), Oxygen Grade (OG), Temperature (T), flux quantity and concentrate composition, the integrated influences of those technology parameters on the sulfur content in bullion, the dust rate and the recovery rate of Pb were analyzed, and the change trends of equilibrium phase composition, oxygen potential and sulfur potential were studied, and the distribution behavior of Pb, Zn, Cu and Fe in each phase were also investigated. Results show that the thermodynamic model calculated values are in good agreement with the Outokumpu semi-industrial test values, and the model can wholly embody the lead flash smelting practice. It's a deliberate result for Outokumpu company, by taking into account the sulfur content in bullion, the dust rate, the recovery rate of Pb and so on, to carry out semi-industrial pilot, while OVPTC is 122 Nm3/t, OG is 95% and smelting temperature is 1210℃.
The copper flash continuous smelting furnace can be regarded as a synthesis reactor of two relatively independent processes:Flash Matting Smelting Process (FMSP) and Copper Continuous Converting Process (CCCP). Based on this thinking, the multi-phase equilibrium model of FMSP and the local-equilibrium model of CCCP were built, and the integrated model of the copper flash continuous smelting process was made up by combinating the above two models with smelting intermediate materials. Then, the multi-factor coupled simulation of the copper flash continuous smelting process was carried out based on the integrated model. The influences of furnace structure, slag type and matte grade on blister formation thermodynamic condition were analyzed, and the change trends of equilibrium phase composition, oxygen potential and sulfur potential were studied, and the integrated influences of the technology parameters, including the Oxygen Volume Per Ton Concentrate (OVPTC), Oxygen Grade (OG), Temperature (T) and concentrate composition, on the sulfur content in blister, Fe3O4 behavior, copper content in slag, recovery rate of Cu, the behavior of Fe and matte were also investigated. Results show that the flash furnace, with double flues and slag partition wall, is an ideal reactor for copper flash continuous smelting, and the recovery rate of copper can be more than 97%.
引文
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