氢在合金熔体中的溶解度与定向凝固多孔铜锰合金的研究
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摘要
金属-气体共晶定向凝固是一种利用气体(主要是氢气)在金属固、液两相中的溶解度差制备规则多孔金属的新工艺,所制得的气孔定向排列在金属中,具有不同于传统多孔金属的性能特点,具有重要的潜在应用价值。从应用角度看,合金比纯金属的适用领域更广,然而以往的大量研究却发现,采用该工艺能够制备得到定向凝固多孔纯金属,却难以得到类似结构的合金。与纯金属相比,制备定向凝固多孔合金主要有两方面的难点,一方面是氢在合金中的溶解度实验数据比较缺乏,也没有可靠的计算模型,难以预测该工艺是否适用于选定合金,另一方面是缺少对合金凝固方式对气孔定向生长影响的研究。本论文针对上述两个方面展开研究。
基于文献数据,总结了氢在不同金属熔体中溶解度的变化规律,提出氢与液态金属原子之间的电子相互作用是决定氢溶解度的主要因素。基于近自由电子理论,建立了计算氢在金属熔体中溶解度的模型。
建立了氢在合金熔体中溶解度的热力学计算模型,改进了模型中多元合金熔体活度系数的计算方法,可以很好地计算氢在多种合金熔体中的溶解度。
采用普通定向凝固工艺,成功制备了定向凝固多孔铜锰合金。实验发现,随着合金试样凝固高度的增加,合金中定向生长气孔的定向性逐渐变差以至最后中断,这种变化由合金的凝固方式决定。进一步发现,当胞晶臂和柱状枝晶一次臂间距远小于定向生长气孔孔径时,以胞状和柱状枝晶方式凝固也可以得到定向生长气孔,而如果变为等轴枝晶方式凝固,则无法得到定向生长气孔。
通过数值模拟,发现随凝固进行,铜锰合金的凝固速度和固-液界面前沿温度梯度都迅速减小,但温度梯度与凝固速度的比值基本保持不变。进一步研究发现,铜锰合金凝固初期为快速胞状凝固。随凝固的进行,合金凝固方式从高速胞状凝固转变为柱状枝晶凝固以及等轴枝晶凝固。通过提高铸型温度和熔体初始温度,可以缩小等轴枝晶凝固的范围,扩大定向生长气孔的区域。实验结果与数值模拟结果相吻合。
Directional solidification of metal-gas eutectic, which is based on the gap of gas (mainly hydrogen) solubility between liquid and solid metals, is a novel process for fabricating regular porous metals with pores aligned in solidification direction. Because of its special property characteristics to that of conventional porous metals, this kind of porous metal has important potential applications. It’s well known that alloys have more application potentials than pure metals. Howerver, it was found in many researches that pure metals with oriented pore structure could be produced successfully by this process, but alloys with similar pore structure could not be made. Comparing with pure metals, two critical difficulties exist in fabrication of directional solidification of porous alloys. One is that there exist neither abundantly documented results nor reliable calculation models for hydrogen solubility of alloys. Therefore, it is difficult to estimate whether an alloy is suitable for this process. The other is that the influence of solidification mode of alloys on growth of oriented pores has not been researched extensively. This thesis will be concentrated on these two aspects.
Variation of hydrogen solubility in different molten metals was summarized based on documented results. It was found that the electron interaction between hydrogen and the molten metal is the most major factor in determining hydrogen solubility in molten metals. According to the nearly-free-electron theory, a model was proposed for calculating hydrogen solubility in molten metals.
Based on an improved method for estimating activity coefficient of multi-component molten alloys, a thermodynamic model was proposed for calculating hydrogen solubility in molten alloys. Calculated results show good agreements with documented experimental results.
Directionally solidified porous Cu-Mn alloy was fabricated successfully by common directional solidification method. It was found that with the increasing of solidification height, oriented pores gradually become irregularly aligned and finally interrupted, which was determined by the solidification mode of the Cu-Mn alloy. Furthermore, it was found that under cellular and columnar dendritic solidification mode, oriented pore structure could also be formed if the cellular and primary dendritic arm spacings are much smaller than the pore diameter. In contrast, when the solidification mode transforms to equiaxed dendritic, no oriented pore structure could be formed.
By numerical simulation, it was found that along with the increasing of solidification height, both solidification velocity and temperature gradient at the solid-liquid interface decrease quickly but their ratio changes little. Furthermore, it was noted that it is a rapid cellular solidification at the beginning of solidification stage, and along with the solidification, the solidification mode transforms from rapid cellular solidification to columnar dendritic solidification and finally equiaxed dendritic solidification. Through increasing the mold preheating temperature and melt pouring temperature, the range of equiaxed dendrite could be decreased and the region of oriented pore structure could be extended, which coincides with experimental results.
基于文献数据,总结了氢在不同金属熔体中溶解度的变化规律,提出氢与液态金属原子之间的电子相互作用是决定氢溶解度的主要因素。基于近自由电子理论,建立了计算氢在金属熔体中溶解度的模型。
建立了氢在合金熔体中溶解度的热力学计算模型,改进了模型中多元合金熔体活度系数的计算方法,可以很好地计算氢在多种合金熔体中的溶解度。
采用普通定向凝固工艺,成功制备了定向凝固多孔铜锰合金。实验发现,随着合金试样凝固高度的增加,合金中定向生长气孔的定向性逐渐变差以至最后中断,这种变化由合金的凝固方式决定。进一步发现,当胞晶臂和柱状枝晶一次臂间距远小于定向生长气孔孔径时,以胞状和柱状枝晶方式凝固也可以得到定向生长气孔,而如果变为等轴枝晶方式凝固,则无法得到定向生长气孔。
通过数值模拟,发现随凝固进行,铜锰合金的凝固速度和固-液界面前沿温度梯度都迅速减小,但温度梯度与凝固速度的比值基本保持不变。进一步研究发现,铜锰合金凝固初期为快速胞状凝固。随凝固的进行,合金凝固方式从高速胞状凝固转变为柱状枝晶凝固以及等轴枝晶凝固。通过提高铸型温度和熔体初始温度,可以缩小等轴枝晶凝固的范围,扩大定向生长气孔的区域。实验结果与数值模拟结果相吻合。
Directional solidification of metal-gas eutectic, which is based on the gap of gas (mainly hydrogen) solubility between liquid and solid metals, is a novel process for fabricating regular porous metals with pores aligned in solidification direction. Because of its special property characteristics to that of conventional porous metals, this kind of porous metal has important potential applications. It’s well known that alloys have more application potentials than pure metals. Howerver, it was found in many researches that pure metals with oriented pore structure could be produced successfully by this process, but alloys with similar pore structure could not be made. Comparing with pure metals, two critical difficulties exist in fabrication of directional solidification of porous alloys. One is that there exist neither abundantly documented results nor reliable calculation models for hydrogen solubility of alloys. Therefore, it is difficult to estimate whether an alloy is suitable for this process. The other is that the influence of solidification mode of alloys on growth of oriented pores has not been researched extensively. This thesis will be concentrated on these two aspects.
Variation of hydrogen solubility in different molten metals was summarized based on documented results. It was found that the electron interaction between hydrogen and the molten metal is the most major factor in determining hydrogen solubility in molten metals. According to the nearly-free-electron theory, a model was proposed for calculating hydrogen solubility in molten metals.
Based on an improved method for estimating activity coefficient of multi-component molten alloys, a thermodynamic model was proposed for calculating hydrogen solubility in molten alloys. Calculated results show good agreements with documented experimental results.
Directionally solidified porous Cu-Mn alloy was fabricated successfully by common directional solidification method. It was found that with the increasing of solidification height, oriented pores gradually become irregularly aligned and finally interrupted, which was determined by the solidification mode of the Cu-Mn alloy. Furthermore, it was found that under cellular and columnar dendritic solidification mode, oriented pore structure could also be formed if the cellular and primary dendritic arm spacings are much smaller than the pore diameter. In contrast, when the solidification mode transforms to equiaxed dendritic, no oriented pore structure could be formed.
By numerical simulation, it was found that along with the increasing of solidification height, both solidification velocity and temperature gradient at the solid-liquid interface decrease quickly but their ratio changes little. Furthermore, it was noted that it is a rapid cellular solidification at the beginning of solidification stage, and along with the solidification, the solidification mode transforms from rapid cellular solidification to columnar dendritic solidification and finally equiaxed dendritic solidification. Through increasing the mold preheating temperature and melt pouring temperature, the range of equiaxed dendrite could be decreased and the region of oriented pore structure could be extended, which coincides with experimental results.
引文
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