无机材料学报 ›› 2024, Vol. 39 ›› Issue (7): 761-768.DOI: 10.15541/jim20230518
收稿日期:
2023-11-06
修回日期:
2024-02-28
出版日期:
2024-07-20
网络出版日期:
2024-03-08
通讯作者:
周益春, 教授. E-mail: yichunzhou@xidian.edu.cn;作者简介:
吴玉豪(2000-), 男, 硕士研究生. E-mail: hsarfr@163.com
基金资助:
WU Yuhao(), PENG Renci, CHENG Chunyu, YANG Li(
), ZHOU Yichun(
)
Received:
2023-11-06
Revised:
2024-02-28
Published:
2024-07-20
Online:
2024-03-08
Contact:
ZHOU Yichun, professor. E-mail: yichunzhou@xidian.edu.cn;About author:
WU Yuhao (2000-), male, Master candidate. E-mail: hsarfr@163.com
Supported by:
摘要:
HfxTa1-xC具有高熔化温度、高硬度、高强度, 以及导电、导热性好等优异性能, 是2000 ℃以上热防护领域极有潜力的候选材料, 但其力学性质与熔化温度随组分变化规律尚不清晰。本研究基于特殊准随机结构(SQS)方法和第一性原理计算, 从共价键强度、价电子浓度(VEC)的微观角度系统地探讨了HfxTa1-xC系固溶体力学性质随组分的变化机理。力学性质计算结果表明: 5种组分(HfC、Hf0.75Ta0.25C、Hf0.5Ta0.5C、Hf0.25Ta0.75C与TaC)中, Hf0.25Ta0.75C固溶体具有最高的弹性模量和剪切模量, 这主要归因于: (1)该组分具有最高的共价键强度; (2)来自C的p轨道和来自Hf或Ta的d轨道之间的特殊键合在VEC=8.75(Hf0.25Ta0.75C)附近被完全填充, 它们强烈抑制形状变化。研究还使用基于从头算分子动力学(AIMD)的分子动力学Z方法计算了HfxTa1-xC系固溶体的熔化曲线。结果显示HfxTa1-xC系固溶体熔化温度反常增加的现象的确存在, 且在Hf0.5Ta0.5C处熔化温度最高(4270 K), 这主要归因于构型熵与共价键强度的协同作用。本研究结果为高熔化温度及高力学性能HfxTa1-xC系固溶体组分的实验选择及其耐高温涂层应用等提供了理论指导, 也为其他过渡金属碳化物研究提供了参考。
中图分类号:
吴玉豪, 彭仁赐, 程春玉, 杨丽, 周益春. HfxTa1-xC体系力学性能及熔化曲线的第一性原理研究[J]. 无机材料学报, 2024, 39(7): 761-768.
WU Yuhao, PENG Renci, CHENG Chunyu, YANG Li, ZHOU Yichun. First-principles Study on Mechanical Properties and Melting Curve of HfxTa1-xC System[J]. Journal of Inorganic Materials, 2024, 39(7): 761-768.
图1 (a) Hf0.75Ta0.25C, (b) Hf0.5Ta0.5C, (c) Hf0.25Ta0.75C, (d) HfC和(e) TaC结构弛豫后得到的稳定结构
Fig. 1 Stable crystal structures after structural relaxation of (a) Hf0.75Ta0.25C, (b) Hf0.5Ta0.5C, (c) Hf0.25Ta0.75C, (d) HfC, and (e) TaC
Compound | Lattice constant/Å | Ecoh/(eV·atom-1) | Emix/(eV·atom-1) |
---|---|---|---|
HfC | a=b=c=9.293 | -10.525 | |
Hf0.75Ta0.25C | a=9.197, b=9.197, c=9.198 | -10.696 | -0.21 |
Hf0.5Ta0.5C | a=9.112, b=9.108, c=9.109 | -10.842 | -0.22 |
Hf0.25Ta0.75C | a=9.034, b=9.034, c=9.023 | -10.977 | -0.15 |
TaC | a=b=c=8.957 | -11.102 |
表S1 HfC、Hf0.75Ta0.25C、Hf0.5Ta0.5C、Hf0.25Ta0.75C、TaC的晶格常数、内聚能(Ecoh)和混合能(Emix)
Table S1 Lattice constants, cohesive enthalpy ( E c o h), and mixing enthalpy ( E m i x ) of HfC, Hf0.75Ta0.25C, Hf0.5Ta0.5C, Hf0.25Ta0.75C and TaC
Compound | Lattice constant/Å | Ecoh/(eV·atom-1) | Emix/(eV·atom-1) |
---|---|---|---|
HfC | a=b=c=9.293 | -10.525 | |
Hf0.75Ta0.25C | a=9.197, b=9.197, c=9.198 | -10.696 | -0.21 |
Hf0.5Ta0.5C | a=9.112, b=9.108, c=9.109 | -10.842 | -0.22 |
Hf0.25Ta0.75C | a=9.034, b=9.034, c=9.023 | -10.977 | -0.15 |
TaC | a=b=c=8.957 | -11.102 |
Compound | C11/GPa | C44/GPa | C12/GPa | |||
---|---|---|---|---|---|---|
This work | Ren et al.[ | This work | Ren et al.[ | This work | Ren et al.[ | |
HfC | 516.2 | 540 | 175.5 | 171 | 102.9 | 112 |
Hf0.75Ta0.25C | 554.1 | 601 | 185.9 | 187 | 114.8 | 117 |
Hf0.5Ta0.5C | 627.2 | 654 | 182.5 | 182 | 108.9 | 120 |
Hf0.25Ta0.75C | 687.8 | 706 | 182.6 | 183 | 120.1 | 124 |
TaC | 679.2 | 674 | 170.9 | 167 | 137.5 | 172 |
表1 HfC、Hf0.75Ta0.25C、Hf0.5Ta0.5C、Hf0.25Ta0.75C、TaC的弹性常数
Table 1 Elastic constants of HfC, Hf0.75Ta0.25C, Hf0.5Ta0.5C, Hf0.25Ta0.75C, and TaC
Compound | C11/GPa | C44/GPa | C12/GPa | |||
---|---|---|---|---|---|---|
This work | Ren et al.[ | This work | Ren et al.[ | This work | Ren et al.[ | |
HfC | 516.2 | 540 | 175.5 | 171 | 102.9 | 112 |
Hf0.75Ta0.25C | 554.1 | 601 | 185.9 | 187 | 114.8 | 117 |
Hf0.5Ta0.5C | 627.2 | 654 | 182.5 | 182 | 108.9 | 120 |
Hf0.25Ta0.75C | 687.8 | 706 | 182.6 | 183 | 120.1 | 124 |
TaC | 679.2 | 674 | 170.9 | 167 | 137.5 | 172 |
图2 HfC、Hf0.75Ta0.25C、Hf0.5Ta0.5C、Hf0.25Ta0.75C和TaC的力学性质变化规律
Fig. 2 Mechanical properties of Hf, Hf0.75Ta0.25C, Hf0.5Ta0.5C, Hf0.25Ta0.75C, and TaC (a) Bulk modulus; (b) Shear modulus; (c) Pugh' ratio; (d) Young's modulus; (e) Hardness
图3 (a) HfxTa1-xC系固溶体的总态密度, 以及(b) TaC, (c) HfC, (d) Hf0.75Ta0.25C, (e) Hf0.5Ta0.5C和(f) Hf0.25Ta0.75C的分态密度
Fig. 3 (a) Total density of states (TDOS) for ternary HfxTa1-xC solid solution, and partial density of states (DOS) for (b) TaC, (c) HfC, (d) Hf0.75Ta0.25C, (e) Hf0.5Ta0.5C, and (f) Hf0.25Ta0.75C Colorful figures are available on website
图S1 HfC的熔化过程示意图
Fig. S1 Schematic diagrams of the melting process of HfC (a) Original stable crystal structure (0 ps); (b) Melting begins (0.1 ps); (c) Complete melting (2.5 ps)
图S3 熔化过程的压力-温度等容曲线
Fig. S3 Pressure-temperature isovolumetric curves during melting process The highest melting point material searched by Bayesian global optimization with deep potential molecular dynamics (a) TaC; (b) HfC; (c) Hf0.75Ta0.25C; (d) Hf0.5Ta0.5C; (e) Hf0.25Ta0.75C
Compound | Pressure/GPa | Melting temperature/K |
---|---|---|
HfC | 14.05 | 3402.1 |
Hf0.75Ta0.25C | 14.82 | 3771.8 |
Hf0.5Ta0.5C | 19.62 | 4720.2 |
Hf0.25Ta0.75C | 19.31 | 4373.0 |
TaC | 22.83 | 4285.3 |
表S2 HfC、Hf0.75Ta0.25C、Hf0.5Ta0.5C、Hf0.25Ta0.75C和TaC的熔化温度及对应的压力
Table S2 Melting temperatures and corresponding pressures of HfC, Hf0.75Ta0.25C, Hf0.5Ta0.5C, Hf0.25Ta0.75C, and TaC
Compound | Pressure/GPa | Melting temperature/K |
---|---|---|
HfC | 14.05 | 3402.1 |
Hf0.75Ta0.25C | 14.82 | 3771.8 |
Hf0.5Ta0.5C | 19.62 | 4720.2 |
Hf0.25Ta0.75C | 19.31 | 4373.0 |
TaC | 22.83 | 4285.3 |
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