Ti（C，N）基金属陶瓷的界面价电子结构与性能研究
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摘要
本文首先应用EET理论系统研究了添加不同碳化物时金属陶瓷陶瓷相的价电子结构以及(Ti,Me)(C,N)/Ni(Co、α-Fe、Fe3Al、FeAl、NiAl)金属陶瓷体系的界面价电子结构,分析了界面价电子结构参数与金属陶瓷力学性能之间的关系。在计算的基础上运用液相烧结技术制备了纳米改性Ti(C,N)基金属陶瓷材料,分析了Ti(C,N)基金属陶瓷的组织、力学性能及热冲击性能。主要内容如下：
首先,介绍了Ti(C,N)基金属陶瓷的发展、制备方法以及成分对组织和力学性能的影响。指出了EET理论的基本原理、研究进展以及应用情况。
其次,运用EET理论和BLD法研究了添加不同碳化物(Mo2C、WC、NbC、TaC、Cr3C2、VC)对金属陶瓷的陶瓷相价电子结构的影响,分析了价电子结构参数(nA)与金属陶瓷材料润湿性(0)以及力学性能(硬度、强韧性)之间的关系。在此基础上计算了(Ti,Me)(C,N)/Ni(Co、α-Fe、Fe3Al、FeAl、NiAl)金属陶瓷体系的界面价电子结构(最强键共价电子数(nA),晶面电子密度(ρ)和界面价电子密度差(Δρ))。研究表明：(1)与WC、NbC、TaC、Cr3C2、VC等碳化物相比,(Ti,Mo)(C,N)/Ni体系界面价电子密度连续性较好；实验证明,Mo2C对Ni/Ti(C,N)金属／陶瓷材料的润湿性的改善作用最为明显。当碳化物添加量为10wt.%时,不同碳化物对润湿性改善程度依次为：Mo2C>TaC>WC>VC>NbC。(2)(Ti,Me)(C,N)(110)/Ni(Co)(110)体系的界面价电子密度差(Δρ)小于10%,即界面价电子连续性好,界面结构稳定；总体来说,金属及金属间化合物对异相界面价电子密度差的影响顺序为(由强到弱)：Ni(Co)>FeAl>α-Fe>Fe3Al>NiAl。(3)综合研究了价电子结构、界面价电子结构与材料强韧性之间的关系,指出采取原位复合制备工艺控制界面结合时,应该尽量在复合材料中存在更多的(110)Ni/(110)C、(110)Co/(110)C等界面,这样使Ti(C,N)基金属陶瓷复合材料具有更优异的综合力学性能。
接下来在基于界面价电子结构计算的基础上,制备了纳米改性Ti(C,N)基金属陶瓷材料样品,研究了其组织、力学性能及抗热冲击性能。结果表明：(1)XRD与SEM分析表明,(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷组织仍为两相结构(陶瓷相+金属相),其中较粗大的陶瓷相颗粒呈明显的芯／壳(core/rim)结构。(2)随着金属相含量的增加(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷的组织更加均匀；而随着Mo含量的增加,金属陶瓷的组织存在着变细的趋势。研究表明,(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷具有优良的力学性能,其硬度值(HRA)达到91.5以上,抗弯强度达到1350MPa以上。(3)就材料的硬度而言,实验结果与价电子结构计算结果是相符的；(4)高温热冲击实验表明：和普通的金属陶瓷相比,纳米改性金属陶瓷的抗热冲击性能较好；随着热冲击循环次数的增加,试样表面的孔洞数量和尺寸都有明显的增加；裂纹在扩展过程中存在弯曲、偏转及桥接现象。
Valence electron structure of ceramic phases in cermets with different carbides and the interface valence electron structure of (Ti,Me) (C,N)/Ni (Co,α-Fe,Fe3Al,FeAl and NiAl) cermets materials were studied systematically by using Empirical Electron Theory in Solid and Molecules (EET theory) and bond length difference (BLD) method in this paper, and the relationship between interface valence electron structure parameters and mechanical properties of Ti(C, N)-based cermets was also studied. Subsequently, nano-modified Ti(C, N)-based cermets samples were prepared by liquid sintering techniques and the microstructure, mechanical properties and thermal shock performance were investigated.
Firstly, the overall development, preparation methods of Ti(C, N)-based cermets and the effect of composition on the microstructure and mechanical properties were introduced. And then basic principles, research progress and application status of Yu's EET theory were described in detail.
Secondly, the author investigated the effect of different carbides on the valence electron structure of complex ceramic phases in Ti(C,N) based cermets and then analyzed the relationship among valence electron structure, wettability and mechanical properties (hardness, strength and toughness) of cermets materials. And the interface valence electron structure parameters including nA(covalent electron number on the strongest bond),p (valence electron density on a specific crystal plane) andΔρ(interface valence electron density difference) were calculated based on the former calculations. The author obtain following results:(1) There is a relatively better continuity of valence electron density of (Ti,Mo)(C,N)/Ni system in comparison with other (Ti,Me)(C,N)/Ni cermets (Me stands for WC,NbC,TaC,Cr3C2 and VC) systems. Virtually, corresponding experiments also prove that Mo2C can play a most effective role in improving the wettability of metal(Ni)on ceramic ((Ti,Mo)(C,N)) and the impact sequence of different carbides on the wettability is Mo2C>TaC>WC>VC>NbC when the content of carbides is 10wt.%. (2) There is a more stable and continuous interface for (Ti,Me) (C,N)(110) /Ni (110) or Co(110) system because the interface valence electron density difference is below 10%.Generally speaking, the impact sequence of different metals or intermetallics on the interface valence electron density difference is Ni(Co)>FeAl>α-Fe>Fe3Al>NiAl. (3) After studying the relationship among valence electron structure, interface valence electron structure and strength&toughness the author pointed out that Ti(C, N) based cermets composites will possess better comprehensive mechanical properties if interfaces such as (110)Ni/(110)C and (110)Co/(110)C can be found or obtained in composites as more as possible as far as in-situ synthesis or preparation technique is concerned.
Subsequently, the author prepared nano-modified Ti(C, N) based cermets samples and investigated the microstructure, mechanical properties and thermal shock properties of the prepared samples based on the above calculations. The following points are noticeable:(1) X-ray diffraction (XRD) and scanning electron microscopy (SEM) studies found that cermets are still composed of ceramic phases and metallic phases and the coarser ceramic particles exhibit so-called core/rim structures. (2) In addition, a more homogeneous microstructure especially the ceramic phase is obtained with the increase of Ni and/or Co contents and the ceramic grains are found to be finer when the content of Mo increases from 5 wt.% to 15 wt.%. Experimental results also show that the mechanical properties are relatively better than common cermets, that is, the hardness (HRA) is above 91.5 and the bend strength is above 1350MPa. (3) As far as the hardness is concerned, the above calculation results agree well with the experimental results. (4) Thermal shock resistance results reveal that nano-modified Ti(C, N) based cermets possesses a better thermal shock resistance in comparison with conventional cermets material. Experiments also reveal that the quantity and size of the voids as well as the size of micro-cracks in cermets increases with thermal shock cycles (N) and the bending, deflection and bridging of thermal cracks are very apparent when thermal cracks propagate in cermets.
首先,介绍了Ti(C,N)基金属陶瓷的发展、制备方法以及成分对组织和力学性能的影响。指出了EET理论的基本原理、研究进展以及应用情况。
其次,运用EET理论和BLD法研究了添加不同碳化物(Mo2C、WC、NbC、TaC、Cr3C2、VC)对金属陶瓷的陶瓷相价电子结构的影响,分析了价电子结构参数(nA)与金属陶瓷材料润湿性(0)以及力学性能(硬度、强韧性)之间的关系。在此基础上计算了(Ti,Me)(C,N)/Ni(Co、α-Fe、Fe3Al、FeAl、NiAl)金属陶瓷体系的界面价电子结构(最强键共价电子数(nA),晶面电子密度(ρ)和界面价电子密度差(Δρ))。研究表明：(1)与WC、NbC、TaC、Cr3C2、VC等碳化物相比,(Ti,Mo)(C,N)/Ni体系界面价电子密度连续性较好；实验证明,Mo2C对Ni/Ti(C,N)金属／陶瓷材料的润湿性的改善作用最为明显。当碳化物添加量为10wt.%时,不同碳化物对润湿性改善程度依次为：Mo2C>TaC>WC>VC>NbC。(2)(Ti,Me)(C,N)(110)/Ni(Co)(110)体系的界面价电子密度差(Δρ)小于10%,即界面价电子连续性好,界面结构稳定；总体来说,金属及金属间化合物对异相界面价电子密度差的影响顺序为(由强到弱)：Ni(Co)>FeAl>α-Fe>Fe3Al>NiAl。(3)综合研究了价电子结构、界面价电子结构与材料强韧性之间的关系,指出采取原位复合制备工艺控制界面结合时,应该尽量在复合材料中存在更多的(110)Ni/(110)C、(110)Co/(110)C等界面,这样使Ti(C,N)基金属陶瓷复合材料具有更优异的综合力学性能。
接下来在基于界面价电子结构计算的基础上,制备了纳米改性Ti(C,N)基金属陶瓷材料样品,研究了其组织、力学性能及抗热冲击性能。结果表明：(1)XRD与SEM分析表明,(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷组织仍为两相结构(陶瓷相+金属相),其中较粗大的陶瓷相颗粒呈明显的芯／壳(core/rim)结构。(2)随着金属相含量的增加(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷的组织更加均匀；而随着Mo含量的增加,金属陶瓷的组织存在着变细的趋势。研究表明,(Ti,Mo,W)(C,N)-Ni-Co金属陶瓷具有优良的力学性能,其硬度值(HRA)达到91.5以上,抗弯强度达到1350MPa以上。(3)就材料的硬度而言,实验结果与价电子结构计算结果是相符的；(4)高温热冲击实验表明：和普通的金属陶瓷相比,纳米改性金属陶瓷的抗热冲击性能较好；随着热冲击循环次数的增加,试样表面的孔洞数量和尺寸都有明显的增加；裂纹在扩展过程中存在弯曲、偏转及桥接现象。
Valence electron structure of ceramic phases in cermets with different carbides and the interface valence electron structure of (Ti,Me) (C,N)/Ni (Co,α-Fe,Fe3Al,FeAl and NiAl) cermets materials were studied systematically by using Empirical Electron Theory in Solid and Molecules (EET theory) and bond length difference (BLD) method in this paper, and the relationship between interface valence electron structure parameters and mechanical properties of Ti(C, N)-based cermets was also studied. Subsequently, nano-modified Ti(C, N)-based cermets samples were prepared by liquid sintering techniques and the microstructure, mechanical properties and thermal shock performance were investigated.
Firstly, the overall development, preparation methods of Ti(C, N)-based cermets and the effect of composition on the microstructure and mechanical properties were introduced. And then basic principles, research progress and application status of Yu's EET theory were described in detail.
Secondly, the author investigated the effect of different carbides on the valence electron structure of complex ceramic phases in Ti(C,N) based cermets and then analyzed the relationship among valence electron structure, wettability and mechanical properties (hardness, strength and toughness) of cermets materials. And the interface valence electron structure parameters including nA(covalent electron number on the strongest bond),p (valence electron density on a specific crystal plane) andΔρ(interface valence electron density difference) were calculated based on the former calculations. The author obtain following results:(1) There is a relatively better continuity of valence electron density of (Ti,Mo)(C,N)/Ni system in comparison with other (Ti,Me)(C,N)/Ni cermets (Me stands for WC,NbC,TaC,Cr3C2 and VC) systems. Virtually, corresponding experiments also prove that Mo2C can play a most effective role in improving the wettability of metal(Ni)on ceramic ((Ti,Mo)(C,N)) and the impact sequence of different carbides on the wettability is Mo2C>TaC>WC>VC>NbC when the content of carbides is 10wt.%. (2) There is a more stable and continuous interface for (Ti,Me) (C,N)(110) /Ni (110) or Co(110) system because the interface valence electron density difference is below 10%.Generally speaking, the impact sequence of different metals or intermetallics on the interface valence electron density difference is Ni(Co)>FeAl>α-Fe>Fe3Al>NiAl. (3) After studying the relationship among valence electron structure, interface valence electron structure and strength&toughness the author pointed out that Ti(C, N) based cermets composites will possess better comprehensive mechanical properties if interfaces such as (110)Ni/(110)C and (110)Co/(110)C can be found or obtained in composites as more as possible as far as in-situ synthesis or preparation technique is concerned.
Subsequently, the author prepared nano-modified Ti(C, N) based cermets samples and investigated the microstructure, mechanical properties and thermal shock properties of the prepared samples based on the above calculations. The following points are noticeable:(1) X-ray diffraction (XRD) and scanning electron microscopy (SEM) studies found that cermets are still composed of ceramic phases and metallic phases and the coarser ceramic particles exhibit so-called core/rim structures. (2) In addition, a more homogeneous microstructure especially the ceramic phase is obtained with the increase of Ni and/or Co contents and the ceramic grains are found to be finer when the content of Mo increases from 5 wt.% to 15 wt.%. Experimental results also show that the mechanical properties are relatively better than common cermets, that is, the hardness (HRA) is above 91.5 and the bend strength is above 1350MPa. (3) As far as the hardness is concerned, the above calculation results agree well with the experimental results. (4) Thermal shock resistance results reveal that nano-modified Ti(C, N) based cermets possesses a better thermal shock resistance in comparison with conventional cermets material. Experiments also reveal that the quantity and size of the voids as well as the size of micro-cracks in cermets increases with thermal shock cycles (N) and the bending, deflection and bridging of thermal cracks are very apparent when thermal cracks propagate in cermets.
引文
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