Fe-Y-B基块体非晶合金的制备、性能与结构
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摘要
由于具有低廉的价格、高机械性能、优异软磁性能和强耐腐蚀性能,Fe基非晶合金备受人们关注。然而,压缩断裂时粉碎性的破坏方式以及铁磁性非晶合金较低的玻璃形成能力,限制了Fe基非晶合金的工业应用。因此,开发兼备优异玻璃形成能力和优良软磁性能的Fe基非晶合金体系具有十分重要的意义。
本文在Fe_(72)Y_68_(22)三元非晶合金的基础上,开发了Fe-M-Y-B(M=Si、Ti、zr、Cr、Al、Co、Ni、w、Mo、Nb)四元块体非晶合金体系。通过微量添加4at.%的Me(Me=W、Mo、Nb)替代Fe,将非晶临界尺寸从2mm提高到4mm或5mm。进一步分析表明:W、Mo和Nb的添加,优化了合金体系内组成元素的原子半径分布,可能形成强化的骨架结构,提高过冷液相的稳定性,从而导致了玻璃形成能力的增强。新开发的Fe-Me-Y-B(Me=W、Mo、Nb)四元铁基块体非晶合金,同时具备了优异的力学性能和良好的软磁性能。比如:Fe_(68)W_4Y_6B_(22)非晶合金的断裂强度达到4011MPa,矫顽力为1.6A/m,饱和磁感应强度为0.77T。
其次,在Fe_(68)Mo_4Y_6B_(22)合金成分的基础上,开发了Fe-Mo-Y-B-M(M=Co、Ni、Ti、zr、Er、Dy、Cr)五元块体非晶合金体系。实验表明:Co、Ni、Ti、Zr、Er和Dy等元素的添加在不同程度上都降低了合金的玻璃形成能力,而微量添加1at.%Cr取代Y,可适当提高合金的玻璃形成能力,通过铜模铸造法成功制备出直径6mm、成分为Fe_(68)Mo_4Y_5Cr_1B_(22)的完全非晶棒。同时,微量Cr的添加也提高了非晶合金在3%NaCl和0.5MNa_2SO_4溶液中的耐腐蚀性能。
此外,结合差示扫描量热分析(DSC)和扩展X射线吸收精细结构(ExtendedX-ray absorption fine structure)分析,仔细阐明了Fe-Mo-Y-B非晶合金奇异玻璃转变行为的微观机理。金属元素(Mo、Y和Fe)和类金属元素(B)之间强烈的相互作用,以及Mo和Y之间存在的相斥作用,共同导致了化学短程有序结构的形成。过冷液相区内的奇异拐点可能是正常玻璃转变的吸热反应与化学短程有序结构进一步演化的放热反应叠加的结果。
利用EXAFS拟合技术,从原子结构的角度探讨了Y微量添加对玻璃形成能力的影响。结果表明:在Fe-Y-B三元合金中,大原子半径元素Y倾向于进入复杂晶体相Fe_(23)B_6中的8c位置,抑制了Fe_3B等简单晶相的析出。当Y含量接近Fe_(23)B_6相中所能提供8c位的最大值时,过多的内应力和晶格畸变导致了Fe_(23)B_6竞争晶体相失稳,增加了凝固过程中过冷液相的稳定性,最终促进了非晶相的形成。
Fe-based metallic glasses have attracted much attention for cheap cost,high mechanical properties,excellent sofimagnetic properties and corrosion resistance. However,their industrial application is largely restricted for intrinsic brittleness or poor glass forming ability(GFA) of ferromagnetic Fe-based metallic glasses.Thus it is important to develop Fe-based bulk metallic glasses(BMGs) with both excellent GFA and good sofimagnetic properties.
First of all,a new quaternary Fe-M-Y-B(M=Si,Ti,Zr,Cr,AI,Co,Ni,W,Mo and Nb) BMGs system was developed on the basis of Fe-Y-B ternary alloy.It is found that minor addition of Me(Me=W,Mo and Nb) enhance GFA largely,which could be attributed to the optimization of atomic radius distribution and the formation of reinforced backbone structure to increase the thermal stability of supercooled liquid. The maximum size of fully glassy rods increases from 2mm for Fe_(72)Y_6B_(22) to 4mm for Fe_(68)W_4Y_6B_(22) and 5ram for Fe_(68)Mo_4Y_6B_(22) and Fe_(68)Nb_4Y_6B(22).Moreover,the new-developed BMGs demonstrate excellent mechanical and good sofimagnetic properties,i.e.,high compression strength of 4011MPa,low coercive force of 1.6A/m and saturated magnetization of 0.77T for Fe_(68)W_4Y_6B_(22) glassy rods.
Secondly,the quinary Fe-Mo-Y-B-M(M=Co,Ni,Ti,Zr,Er,Dy and Cr) BMGs alloy system was developed based on the composition of Fe_(68)Mo_4Y_6B_(22).It is found that minor addition of all these elements except for Cr deteriorates the GFA in the investigated composition range,while the substitution of 1at.%Cr for Y enhance the GFA.Using copper mould casting,glassy cylindrical rods with 6mm in diameter were successfully synthesized with the nominal composition of Fe_(68)Mo_4Cr_1Y_5B_(22).At the same time,minor addition of Cr is capable of improving the corrosion resistance of glassy alloy in 3%NaCI and 0.5M Na_2SO_4 solution.
Additionally,anomalous glass transition in the supercooled liquid region of Fe-Mo-Y-B BMGs was carefully elucidated using differential scanning calorimetry (DSC) and extended X-ray absorption fine structure(EXAFS) methods.It is concluded that the anomalous inflection could be due to the overlapping of endothermic peak characteristic of glass transition and exothermal peak characteristic of structural evolution of chemical short-range ordering.The chemical short-range ordering might be attributed to strong interaction between metal atoms(Mo,Y and Fe) and metalloid atoms(B),combined with repulsive force between Mo and Y.
From the aspect of local atomic structure,the effect of minor Y addition on the glass formation ability was investigated utilizing EXAFS simulation.It is proposed that in Fe-Y-B ternay alloy,Y atoms with large atomic radius tend to occupy the 8c site in complex Fe_(23)B_6 structure and constrain the precipitation of simple crystalline phase,i.e.,FeaB.When Y content is close to the maximum value of 8c site provided by Fe_(23)B_6,excessive internal stress and lattice distortion introduced by Y atoms might lead to the instability of Fe_(23)B_6 competition crystalline phase and enhance the stability of supercooled liquid,eventually favoring the formation of amorphous state during solidification.
本文在Fe_(72)Y_68_(22)三元非晶合金的基础上,开发了Fe-M-Y-B(M=Si、Ti、zr、Cr、Al、Co、Ni、w、Mo、Nb)四元块体非晶合金体系。通过微量添加4at.%的Me(Me=W、Mo、Nb)替代Fe,将非晶临界尺寸从2mm提高到4mm或5mm。进一步分析表明:W、Mo和Nb的添加,优化了合金体系内组成元素的原子半径分布,可能形成强化的骨架结构,提高过冷液相的稳定性,从而导致了玻璃形成能力的增强。新开发的Fe-Me-Y-B(Me=W、Mo、Nb)四元铁基块体非晶合金,同时具备了优异的力学性能和良好的软磁性能。比如:Fe_(68)W_4Y_6B_(22)非晶合金的断裂强度达到4011MPa,矫顽力为1.6A/m,饱和磁感应强度为0.77T。
其次,在Fe_(68)Mo_4Y_6B_(22)合金成分的基础上,开发了Fe-Mo-Y-B-M(M=Co、Ni、Ti、zr、Er、Dy、Cr)五元块体非晶合金体系。实验表明:Co、Ni、Ti、Zr、Er和Dy等元素的添加在不同程度上都降低了合金的玻璃形成能力,而微量添加1at.%Cr取代Y,可适当提高合金的玻璃形成能力,通过铜模铸造法成功制备出直径6mm、成分为Fe_(68)Mo_4Y_5Cr_1B_(22)的完全非晶棒。同时,微量Cr的添加也提高了非晶合金在3%NaCl和0.5MNa_2SO_4溶液中的耐腐蚀性能。
此外,结合差示扫描量热分析(DSC)和扩展X射线吸收精细结构(ExtendedX-ray absorption fine structure)分析,仔细阐明了Fe-Mo-Y-B非晶合金奇异玻璃转变行为的微观机理。金属元素(Mo、Y和Fe)和类金属元素(B)之间强烈的相互作用,以及Mo和Y之间存在的相斥作用,共同导致了化学短程有序结构的形成。过冷液相区内的奇异拐点可能是正常玻璃转变的吸热反应与化学短程有序结构进一步演化的放热反应叠加的结果。
利用EXAFS拟合技术,从原子结构的角度探讨了Y微量添加对玻璃形成能力的影响。结果表明:在Fe-Y-B三元合金中,大原子半径元素Y倾向于进入复杂晶体相Fe_(23)B_6中的8c位置,抑制了Fe_3B等简单晶相的析出。当Y含量接近Fe_(23)B_6相中所能提供8c位的最大值时,过多的内应力和晶格畸变导致了Fe_(23)B_6竞争晶体相失稳,增加了凝固过程中过冷液相的稳定性,最终促进了非晶相的形成。
Fe-based metallic glasses have attracted much attention for cheap cost,high mechanical properties,excellent sofimagnetic properties and corrosion resistance. However,their industrial application is largely restricted for intrinsic brittleness or poor glass forming ability(GFA) of ferromagnetic Fe-based metallic glasses.Thus it is important to develop Fe-based bulk metallic glasses(BMGs) with both excellent GFA and good sofimagnetic properties.
First of all,a new quaternary Fe-M-Y-B(M=Si,Ti,Zr,Cr,AI,Co,Ni,W,Mo and Nb) BMGs system was developed on the basis of Fe-Y-B ternary alloy.It is found that minor addition of Me(Me=W,Mo and Nb) enhance GFA largely,which could be attributed to the optimization of atomic radius distribution and the formation of reinforced backbone structure to increase the thermal stability of supercooled liquid. The maximum size of fully glassy rods increases from 2mm for Fe_(72)Y_6B_(22) to 4mm for Fe_(68)W_4Y_6B_(22) and 5ram for Fe_(68)Mo_4Y_6B_(22) and Fe_(68)Nb_4Y_6B(22).Moreover,the new-developed BMGs demonstrate excellent mechanical and good sofimagnetic properties,i.e.,high compression strength of 4011MPa,low coercive force of 1.6A/m and saturated magnetization of 0.77T for Fe_(68)W_4Y_6B_(22) glassy rods.
Secondly,the quinary Fe-Mo-Y-B-M(M=Co,Ni,Ti,Zr,Er,Dy and Cr) BMGs alloy system was developed based on the composition of Fe_(68)Mo_4Y_6B_(22).It is found that minor addition of all these elements except for Cr deteriorates the GFA in the investigated composition range,while the substitution of 1at.%Cr for Y enhance the GFA.Using copper mould casting,glassy cylindrical rods with 6mm in diameter were successfully synthesized with the nominal composition of Fe_(68)Mo_4Cr_1Y_5B_(22).At the same time,minor addition of Cr is capable of improving the corrosion resistance of glassy alloy in 3%NaCI and 0.5M Na_2SO_4 solution.
Additionally,anomalous glass transition in the supercooled liquid region of Fe-Mo-Y-B BMGs was carefully elucidated using differential scanning calorimetry (DSC) and extended X-ray absorption fine structure(EXAFS) methods.It is concluded that the anomalous inflection could be due to the overlapping of endothermic peak characteristic of glass transition and exothermal peak characteristic of structural evolution of chemical short-range ordering.The chemical short-range ordering might be attributed to strong interaction between metal atoms(Mo,Y and Fe) and metalloid atoms(B),combined with repulsive force between Mo and Y.
From the aspect of local atomic structure,the effect of minor Y addition on the glass formation ability was investigated utilizing EXAFS simulation.It is proposed that in Fe-Y-B ternay alloy,Y atoms with large atomic radius tend to occupy the 8c site in complex Fe_(23)B_6 structure and constrain the precipitation of simple crystalline phase,i.e.,FeaB.When Y content is close to the maximum value of 8c site provided by Fe_(23)B_6,excessive internal stress and lattice distortion introduced by Y atoms might lead to the instability of Fe_(23)B_6 competition crystalline phase and enhance the stability of supercooled liquid,eventually favoring the formation of amorphous state during solidification.
引文
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