基于合金化改善镁合金强/韧性的研究
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摘要
针对当前镁合金力学性能不能满足应用需求,可用合金选择性少,以及稀土系镁合金成本高的问题,本文探索新的镁合金强/韧化设计新思路,期望通过寻找新的合金元素开发出具有高强/高韧性能的新型镁合金。
作者总结了24种合金元素的原子信息,提出镁合金强/韧化设计思路:
1.在镁合金中添加难溶性合金元素,生成具有高熔点高硬度金属间化合物,提高镁合金孪生变形的临界剪切应力,阻碍变形过程中的晶界滑移提高强度。根据相图和原子信息,选择Sb和Ge元素验证设计思路的可行性。
2.从材料设计的角度分析镁合金的强韧化问题,根据原子团簇理论和金属键强弱的影响因素,选择Ga元素进行合金化,开发Mg-Ga系镁合金。
合金熔炼与制备采用金属模铸造法,分别进行了铸态Mg-Sb二元合金中α-Mg_3Sb_2相形态变化的研究,AZ31 Sb合金化后α-Mg_3Sb_2相的形态及其对合金显微组织和性能影响的研究;铸态Mg-Ge二元合金中Mg_2Ge相的形态及其对合金显微组织与性能研究,铸态AZ31 Ge合金化Mg_2Ge形态对合金显微组织与性能影响的研究,Al和Zn对Mg_2Ge金属间化合物形貌的影响;Mg-Ga二元合金显微组织与性能的研究和Mg-xGa-3Al-1Zn系合金显微组织与性能的研究。
Sb合金化结果表明:由于存在较大的电负数差,Sb元素与Mg元素之间具有较强的结合力,两种原子相遇会发生电子转移,形成固溶有Mg的离子晶体α-Mg_3Sb_2。在熔炼Mg-10(wt.%)Sb合金时,熔体中形成大量α-Mg_3Sb_2,其较大的密度导致熔体分层,得到成分相差较大的Mg-9(wt.%)Sb和Mg-13(wt.%)Sb双层合金铸锭。因此镁合金中只能添加少量的Sb。α-Mg_3Sb_2金属间化合物在Mg-9(wt.%)Sb合金中有针棒状和矩形块状两种形态,在Mg-13(wt.%)Sb中呈矩形块状。AZ31进行Sb合金化时发现,Sb对合金没有晶粒细化作用;α-Mg_3Sb_2析出相在铸态AZ31中呈针棒状,均匀分布在基体内。拉伸实验结果表明,少量的针棒状α-Mg_3Sb_2析出相的存在对镁合金抗拉强度影响不大,随着该析出相体积分数的增加,抗拉强度略有下降,但仍然具有较高的韧性。在应力-应变曲线上观察到了晶粒发生孪生变形时产生的应力释放现象。
Ge合金化结果表明:Ge对镁及镁合金有晶粒细化作用,析出相Mg_2Ge的形态受合金元素影响很大,析出相的形态影响合金的拉伸性能。在Mg-Ge二元合金中,析出相Mg_2Ge呈针棒状,形成(α-Mg+Mg_2Ge)共晶分布在晶界上,对镁有强化作用。铸态AZ31中Mg_2Ge相呈汉字状,不利于合金力学性能。Mg-Zn-Ge和Mg-3Al-Ge显微组织表明,Al和Zn对Mg_2Ge相从针棒状向汉字状转变都有影响。因此,控制析出相Mg_2Ge的形态成为Ge改善镁合金强韧性的关键。
Mg-Ga二元合金实验表明:固溶的Ga元素可以显著降低α-Mg晶格常数和平均原子间距,Ga还可以有效的细化镁合金晶粒,显著提高纯镁的韧性、屈服强度和极限拉伸强度。Mg_5Ga_2析出相在铸态组织中的形态和分布与Ga含量有关,Ga含量较低时,Mg_5Ga_2析出相呈颗粒状均匀分布在基体内;Ga含量较高时,一部分Mg_5Ga_2析出相呈块状或孤岛状分布在晶界处。固溶处理可以有效提高Ga在Mg中的固溶度,时效处理可使合金中析出直径小于100 nm的针棒状Mg_5Ga_2,该析出相最先从晶界处析出,随着时效时间的延长逐渐向晶内扩展,合金的屈服强度也随时效时间的延长而逐渐增加。
Mg-xGa-3Al-1Zn系合金的研究结果表明:Ga细化了合金的晶粒,Mg_5Ga_2析出相的形态和分布规律与Mg-Ga二元合金相似。固溶处理后Mg_5Ga_2析出相显著减少,合金韧性较好,Mg-4.5Ga-3Al-1Zn合金的延伸率达到11.7%。时效处理效果与Mg-Ga二元合金基本相同,Mg-4.5Ga-3Al-1Zn合金的极限拉伸强度最高达到207 MPa。Al和Zn元素可以加速Mg_5Ga_2强化相的析出。
Ga合金化研究结果证实,根据团簇理论和增强原子结合力的设计思想,寻找新的能够提高镁合金强度/韧性的合金元素的思路可行,Mg-Ga系镁合金具有开发成为新型高强镁合金的潜力。
最后,作者还通过对Ga、Al、Zn、Mn、Li、Sn、Si、Sb和Ge等非稀土系元素的特征进行综合分析,总结出可以强/韧化镁合金的非稀土系合金元素所具有的一般特征:
(1)合金元素可以固溶于镁基体中;
(2)合金元素的原子半径都小于Mg原子半径;
(3)合金元素的化合价应尽可能高;
(4)合金元素的电负数应该小于1.9。
The application of Magnesium alloys is dramatically limited by the low mechanical properties, few alloys systems and the high cost of Rare earth Magnesium alloys. Author wants to find new alloying element and supply a new strengthening design method of Mg alloys.
Author summarized atomic information of 24 type of alloying elements including Magnesium element. Both methods of alloying of magnesium alloys were supposed according to the strengthening mechanism. The both methods were followed:
(1) Indissolvable elements in Magnesium alloys were added to Magnesium alloys in order to improve the critical shearing stress of twin and oppose the grain boundary slipping in deformation process. However, the ductility of magnesium alloys was reduced. According to the phase diagrams and atomic information, Antimony and Germanium were selected and experimented to prove practical in practice.
(2) The strengthening of Magnesium alloys was researched from the subjedt of material design and Gallium was chosen according to the electron concentration and the influencing factors of metallic bond. This is a new method for strengthening the Magnesium alloys.
The dissertation included morphology ofα-Mg_3Sb_2 precipitates in Mg-Sb binary alloys, microstructure and mechanical properties of AZ31 with the addition of Sb; Microstructure evolution and mechanical properties of as-cast Mg-Ge binary magnesium alloys, Microstructure and mechanical property of as-cast AZ31 with the addition of Germanium, the effect of Al and Zn on the morphology of Mg_2Ge in Mg alloys, microstructure and mechanical properties of Mg-Ga binary alloys and the microstructure and mechanical properties of Mg-xGa-3Al-Zn alloys. All of the alloy ingots were prepared by die casting.
The results of Sb alloying of Mg alloys indicated that the intermetallic compoundα-Mg_3Sb_2 soluted with many Mg atoms because of the difference between Pauling electro-negativity values of them. A double layer alloy ingot with Mg-9(wt.%)Sb and Mg-13(wt.%)Sb was gotten when the Mg-10(wt.%)Sb was prepared because a large number of theα-Mg_3Sb_2 grains with high density were synthesized and some of them deposited on the bottom of crucible. Then the amount of the addition of Sb to Magnesium alloys was limited. Theα-Mg_3Sb_2 precipitates were rectangle block in as-cast Mg-13(wt.%)Sb alloy while in as-cast Mg-9(wt.%)Sb alloy majority of them were rod shape and minority were rectangle block. The experiment results of AZ31 with the addition of Sb indicated the rod-shaped intermetallic compoundα-Mg_3Sb_2 formed and distributed homogenously in substrate. The elongations of alloys with Sb addition are good (δ>10%). Both of tensile strength and elongation of alloys appreciably reduce with the increase of contents of Sb in alloys. Twin deforming and boundary sliding are the main deformation of AZ31 with and without Sb addition.
The results of Ge alloying of Mg alloys indicated that Ge could refine the Mg alloys, the morphologies of Mg_2Ge precipitates reduced the tensile properties of Mg alloys and were affected by other alloying elements in Mg alloys. The Mg_2Ge precipitates in Mg-Ge binary alloys were rod-shaped and formed the eutectic of (α-Mg + Mg_2Ge) which could effectively enhance the grain boundaries ofα-Mg. In the microstructure of as-cast AZ31 with the addition of Ge, the Mg_2Ge intermetallic compound presented Chinese script, which reduced the tensile properties of alloys. The microstructure of as-cast Mg-3Al-Ge and as-cast Mg-1Zn-Ge alloys indicated that both of Al and Zn elements could affect the morphology of Mg_2Ge.
The experiment results of Mg-Ga binary alloys presented that Ga dissolved in Mg alloys dramatically reduced the lattice parameters and the average distance between of atoms ofα-Mg grains, the tensile properties of pure Mg were improved dramtically. The morphology and distribution of Mg_5Ga_2 in as-cast Mg-Ga binary alloys were associated with the content of Ga. If the content of Ga was below the 1.5 at.% (included) in as-cast alloys, the Mg_5Ga_2 precipitates were particles and homogeously distributed in matrix. If the content of Ga was above 2.0 at.% (included) in as-cast alloys, the Mg_5Ga_2 precipitates were block and distributed on grain boundaries. The solid solubility of Ga in Mg-xGa binary alloy could be improved by solution treatment. A lot of tiny rod-shaped Mg_5Ga_2 precipitates (φ<100 nm) were precipitated in aging treatment and the yield tensile strengthed of the alloys was improved.
In as-cast Mg-xGa-3Al-1Zn alloys the morphology and distribution of Mg_5Ga_2 precipitates were similar with the rule of them in as-cast Mg-Ga binary alloys. The elongations of Mg-xGa-3Al-1Zn alloys were better after solution treatment. The effects of aging treatment on Mg-xGa-3Al-lZn alloys were similar with it on Mg-Ga binary alloys. The ultimate tensile strengthen of Mg-4.5Ga-3Al-1Zn alloy was higher, 207 MPa after aging treatment. The aging microstructure of Mg-xGa-3Al-1Zn alloys indicated both Al and Zn could accelerate the precipitation of Mg_5Ga_2 phase. The Mg-Ga system alloys should be further study to tap the potential and develop new Magnesium alloys with high performance.
The Ga alloying results of Mg alloy proved that the atom cluster theory and the influencing factors of metallic bond were useful to find new alloying elements to strength Mg alloys and the Mg-Ga system alloys have large potentiality to be developed new high performance Mg alloys.
At last, general characters of magnesium alloying elements except for Rare earth elements were summarized according to Ga, Al, Zn, Mn, Li, Sn, Si, Sb and Ge elements. The contents of the principle were followed:
(1) The alloying elements could be dissolved in Mg alloys even at ambient temperature;
(2) The radius of them should be much smaller than that of Mg atom;
(3) The charge of basic ion of them should be more;
(4) The Pauling electro-negativity values of them should be smaller than 1.9.
作者总结了24种合金元素的原子信息,提出镁合金强/韧化设计思路:
1.在镁合金中添加难溶性合金元素,生成具有高熔点高硬度金属间化合物,提高镁合金孪生变形的临界剪切应力,阻碍变形过程中的晶界滑移提高强度。根据相图和原子信息,选择Sb和Ge元素验证设计思路的可行性。
2.从材料设计的角度分析镁合金的强韧化问题,根据原子团簇理论和金属键强弱的影响因素,选择Ga元素进行合金化,开发Mg-Ga系镁合金。
合金熔炼与制备采用金属模铸造法,分别进行了铸态Mg-Sb二元合金中α-Mg_3Sb_2相形态变化的研究,AZ31 Sb合金化后α-Mg_3Sb_2相的形态及其对合金显微组织和性能影响的研究;铸态Mg-Ge二元合金中Mg_2Ge相的形态及其对合金显微组织与性能研究,铸态AZ31 Ge合金化Mg_2Ge形态对合金显微组织与性能影响的研究,Al和Zn对Mg_2Ge金属间化合物形貌的影响;Mg-Ga二元合金显微组织与性能的研究和Mg-xGa-3Al-1Zn系合金显微组织与性能的研究。
Sb合金化结果表明:由于存在较大的电负数差,Sb元素与Mg元素之间具有较强的结合力,两种原子相遇会发生电子转移,形成固溶有Mg的离子晶体α-Mg_3Sb_2。在熔炼Mg-10(wt.%)Sb合金时,熔体中形成大量α-Mg_3Sb_2,其较大的密度导致熔体分层,得到成分相差较大的Mg-9(wt.%)Sb和Mg-13(wt.%)Sb双层合金铸锭。因此镁合金中只能添加少量的Sb。α-Mg_3Sb_2金属间化合物在Mg-9(wt.%)Sb合金中有针棒状和矩形块状两种形态,在Mg-13(wt.%)Sb中呈矩形块状。AZ31进行Sb合金化时发现,Sb对合金没有晶粒细化作用;α-Mg_3Sb_2析出相在铸态AZ31中呈针棒状,均匀分布在基体内。拉伸实验结果表明,少量的针棒状α-Mg_3Sb_2析出相的存在对镁合金抗拉强度影响不大,随着该析出相体积分数的增加,抗拉强度略有下降,但仍然具有较高的韧性。在应力-应变曲线上观察到了晶粒发生孪生变形时产生的应力释放现象。
Ge合金化结果表明:Ge对镁及镁合金有晶粒细化作用,析出相Mg_2Ge的形态受合金元素影响很大,析出相的形态影响合金的拉伸性能。在Mg-Ge二元合金中,析出相Mg_2Ge呈针棒状,形成(α-Mg+Mg_2Ge)共晶分布在晶界上,对镁有强化作用。铸态AZ31中Mg_2Ge相呈汉字状,不利于合金力学性能。Mg-Zn-Ge和Mg-3Al-Ge显微组织表明,Al和Zn对Mg_2Ge相从针棒状向汉字状转变都有影响。因此,控制析出相Mg_2Ge的形态成为Ge改善镁合金强韧性的关键。
Mg-Ga二元合金实验表明:固溶的Ga元素可以显著降低α-Mg晶格常数和平均原子间距,Ga还可以有效的细化镁合金晶粒,显著提高纯镁的韧性、屈服强度和极限拉伸强度。Mg_5Ga_2析出相在铸态组织中的形态和分布与Ga含量有关,Ga含量较低时,Mg_5Ga_2析出相呈颗粒状均匀分布在基体内;Ga含量较高时,一部分Mg_5Ga_2析出相呈块状或孤岛状分布在晶界处。固溶处理可以有效提高Ga在Mg中的固溶度,时效处理可使合金中析出直径小于100 nm的针棒状Mg_5Ga_2,该析出相最先从晶界处析出,随着时效时间的延长逐渐向晶内扩展,合金的屈服强度也随时效时间的延长而逐渐增加。
Mg-xGa-3Al-1Zn系合金的研究结果表明:Ga细化了合金的晶粒,Mg_5Ga_2析出相的形态和分布规律与Mg-Ga二元合金相似。固溶处理后Mg_5Ga_2析出相显著减少,合金韧性较好,Mg-4.5Ga-3Al-1Zn合金的延伸率达到11.7%。时效处理效果与Mg-Ga二元合金基本相同,Mg-4.5Ga-3Al-1Zn合金的极限拉伸强度最高达到207 MPa。Al和Zn元素可以加速Mg_5Ga_2强化相的析出。
Ga合金化研究结果证实,根据团簇理论和增强原子结合力的设计思想,寻找新的能够提高镁合金强度/韧性的合金元素的思路可行,Mg-Ga系镁合金具有开发成为新型高强镁合金的潜力。
最后,作者还通过对Ga、Al、Zn、Mn、Li、Sn、Si、Sb和Ge等非稀土系元素的特征进行综合分析,总结出可以强/韧化镁合金的非稀土系合金元素所具有的一般特征:
(1)合金元素可以固溶于镁基体中;
(2)合金元素的原子半径都小于Mg原子半径;
(3)合金元素的化合价应尽可能高;
(4)合金元素的电负数应该小于1.9。
The application of Magnesium alloys is dramatically limited by the low mechanical properties, few alloys systems and the high cost of Rare earth Magnesium alloys. Author wants to find new alloying element and supply a new strengthening design method of Mg alloys.
Author summarized atomic information of 24 type of alloying elements including Magnesium element. Both methods of alloying of magnesium alloys were supposed according to the strengthening mechanism. The both methods were followed:
(1) Indissolvable elements in Magnesium alloys were added to Magnesium alloys in order to improve the critical shearing stress of twin and oppose the grain boundary slipping in deformation process. However, the ductility of magnesium alloys was reduced. According to the phase diagrams and atomic information, Antimony and Germanium were selected and experimented to prove practical in practice.
(2) The strengthening of Magnesium alloys was researched from the subjedt of material design and Gallium was chosen according to the electron concentration and the influencing factors of metallic bond. This is a new method for strengthening the Magnesium alloys.
The dissertation included morphology ofα-Mg_3Sb_2 precipitates in Mg-Sb binary alloys, microstructure and mechanical properties of AZ31 with the addition of Sb; Microstructure evolution and mechanical properties of as-cast Mg-Ge binary magnesium alloys, Microstructure and mechanical property of as-cast AZ31 with the addition of Germanium, the effect of Al and Zn on the morphology of Mg_2Ge in Mg alloys, microstructure and mechanical properties of Mg-Ga binary alloys and the microstructure and mechanical properties of Mg-xGa-3Al-Zn alloys. All of the alloy ingots were prepared by die casting.
The results of Sb alloying of Mg alloys indicated that the intermetallic compoundα-Mg_3Sb_2 soluted with many Mg atoms because of the difference between Pauling electro-negativity values of them. A double layer alloy ingot with Mg-9(wt.%)Sb and Mg-13(wt.%)Sb was gotten when the Mg-10(wt.%)Sb was prepared because a large number of theα-Mg_3Sb_2 grains with high density were synthesized and some of them deposited on the bottom of crucible. Then the amount of the addition of Sb to Magnesium alloys was limited. Theα-Mg_3Sb_2 precipitates were rectangle block in as-cast Mg-13(wt.%)Sb alloy while in as-cast Mg-9(wt.%)Sb alloy majority of them were rod shape and minority were rectangle block. The experiment results of AZ31 with the addition of Sb indicated the rod-shaped intermetallic compoundα-Mg_3Sb_2 formed and distributed homogenously in substrate. The elongations of alloys with Sb addition are good (δ>10%). Both of tensile strength and elongation of alloys appreciably reduce with the increase of contents of Sb in alloys. Twin deforming and boundary sliding are the main deformation of AZ31 with and without Sb addition.
The results of Ge alloying of Mg alloys indicated that Ge could refine the Mg alloys, the morphologies of Mg_2Ge precipitates reduced the tensile properties of Mg alloys and were affected by other alloying elements in Mg alloys. The Mg_2Ge precipitates in Mg-Ge binary alloys were rod-shaped and formed the eutectic of (α-Mg + Mg_2Ge) which could effectively enhance the grain boundaries ofα-Mg. In the microstructure of as-cast AZ31 with the addition of Ge, the Mg_2Ge intermetallic compound presented Chinese script, which reduced the tensile properties of alloys. The microstructure of as-cast Mg-3Al-Ge and as-cast Mg-1Zn-Ge alloys indicated that both of Al and Zn elements could affect the morphology of Mg_2Ge.
The experiment results of Mg-Ga binary alloys presented that Ga dissolved in Mg alloys dramatically reduced the lattice parameters and the average distance between of atoms ofα-Mg grains, the tensile properties of pure Mg were improved dramtically. The morphology and distribution of Mg_5Ga_2 in as-cast Mg-Ga binary alloys were associated with the content of Ga. If the content of Ga was below the 1.5 at.% (included) in as-cast alloys, the Mg_5Ga_2 precipitates were particles and homogeously distributed in matrix. If the content of Ga was above 2.0 at.% (included) in as-cast alloys, the Mg_5Ga_2 precipitates were block and distributed on grain boundaries. The solid solubility of Ga in Mg-xGa binary alloy could be improved by solution treatment. A lot of tiny rod-shaped Mg_5Ga_2 precipitates (φ<100 nm) were precipitated in aging treatment and the yield tensile strengthed of the alloys was improved.
In as-cast Mg-xGa-3Al-1Zn alloys the morphology and distribution of Mg_5Ga_2 precipitates were similar with the rule of them in as-cast Mg-Ga binary alloys. The elongations of Mg-xGa-3Al-1Zn alloys were better after solution treatment. The effects of aging treatment on Mg-xGa-3Al-lZn alloys were similar with it on Mg-Ga binary alloys. The ultimate tensile strengthen of Mg-4.5Ga-3Al-1Zn alloy was higher, 207 MPa after aging treatment. The aging microstructure of Mg-xGa-3Al-1Zn alloys indicated both Al and Zn could accelerate the precipitation of Mg_5Ga_2 phase. The Mg-Ga system alloys should be further study to tap the potential and develop new Magnesium alloys with high performance.
The Ga alloying results of Mg alloy proved that the atom cluster theory and the influencing factors of metallic bond were useful to find new alloying elements to strength Mg alloys and the Mg-Ga system alloys have large potentiality to be developed new high performance Mg alloys.
At last, general characters of magnesium alloying elements except for Rare earth elements were summarized according to Ga, Al, Zn, Mn, Li, Sn, Si, Sb and Ge elements. The contents of the principle were followed:
(1) The alloying elements could be dissolved in Mg alloys even at ambient temperature;
(2) The radius of them should be much smaller than that of Mg atom;
(3) The charge of basic ion of them should be more;
(4) The Pauling electro-negativity values of them should be smaller than 1.9.
引文
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